阅读说明：本技术 一种纳米氧化铜-石墨相氮化碳复合材料的制备方法及其制备用干燥装置 (Preparation method of nano copper oxide-graphite phase carbon nitride composite material and drying device for preparation ) 是由 高晓红 王彦明 李萍 于 2021-09-25 设计创作，主要内容包括：本发明公开了一种纳米氧化铜-石墨相氮化碳复合材料的制备方法及其制备用干燥装置,通过按比例称取三聚氰胺或二聚氰胺,以及硝酸铜,加入溶剂中进行搅拌,然后通过干燥装置进行蒸发干燥,将干燥得到的固体研磨后放入加热炉中煅烧,可得纳米CuO@g-C3N4复合材料。本发明的制备方法成本低,操作简便,适用于规模化批量生产,所得产物粒度较小,氮化碳复合材料晶面间距较大,层间结合力更弱；干燥装置采用多蒸馏瓶层叠设计,生产效率高,整体占用空间小,通过搅拌组件可防止蒸馏瓶内的溶剂进入到蒸发管和收集瓶内,提高蒸发速度,通过柔性出水头将热水淋至蒸馏瓶上部,使得蒸馏瓶全瓶身均能接触热水,提高蒸发速度。(The invention discloses a preparation method of a nano copper oxide-graphite phase carbon nitride composite material and a drying device for preparation, wherein melamine or dicyandiamide and copper nitrate are weighed according to a proportion, added into a solvent for stirring, then evaporated and dried by the drying device, and the dried solid is ground and then put into a heating furnace for calcination, so that the nano CuO @ g-C3N4 composite material is obtained. The preparation method has low cost and simple and convenient operation, is suitable for large-scale batch production, and the obtained product has smaller granularity, larger crystal spacing of the carbon nitride composite material and weaker interlayer bonding force; drying device adopts the range upon range of design of many distillation flasks, and production efficiency is high, and whole occupation space is little, can prevent through the stirring subassembly that the solvent in the distillation flask from entering into in evaporating pipe and the receiving flask, improves the evaporation rate, drenches hot water to distillation flask upper portion through flexible play faucet for the whole body homoenergetic of distillation flask contacts hot water, improves the evaporation rate.)

1. A preparation method of a nano copper oxide-graphite phase carbon nitride composite material is characterized by comprising the following steps:

weighing the first raw material and the second raw material according to the weight ratio of (2-7) to 1, adding the first raw material and the second raw material into a solvent, stirring, and then evaporating and drying through a drying device; wherein the first raw material is melamine or dicyandiamide, and the second raw material is copper nitrate;

and grinding the dried solid, putting the ground solid into a container, putting the container into a heating furnace, controlling the temperature at 500-550 ℃, and calcining for 3-5 hours to obtain the nano CuO @ g-C3N4 composite material.

2. The method of preparing a nano copper oxide-graphite phase carbon nitride composite material according to claim 1, wherein the solvent is a mixture of one or more of acetone, ethanol and water.

3. The method for preparing a nano copper oxide-graphite phase carbon nitride composite material according to claim 1, wherein the container is a quartz crucible and the heating furnace is a tubular heating furnace.

4. The method for preparing a nano copper oxide-graphite phase carbon nitride composite material according to claim 1, wherein nitrogen protection is used in the calcination process, and the flow rate of the nitrogen protection gas is 0.4L/min.

5. The drying device for preparing the nano copper oxide-graphite phase carbon nitride composite material according to claim 1, comprising a frame (5), and a rotary evaporation system (1), a condensation system (2), a first lifting mechanism (3) and a second lifting mechanism (4) which are installed on the frame (5), wherein:

the condensing system (2) comprises a condenser (21) and a collecting bottle (22), and the lower end of the condenser (21) is sleeved with the collecting bottle (22);

the rotary evaporation system (1) comprises a rotary driving mechanism (11), a circulating water heating mechanism (12) and at least two evaporation mechanisms (6), wherein the rotary driving mechanism (11) comprises a driving shell (111) arranged at the lifting end of the first lifting mechanism (3), and a driving motor (112) is arranged on the driving shell (111);

the evaporation mechanism (6) comprises a distillation flask (61), an evaporation tube (62), a feeding tube (63), a stirring mechanism (64), a transmission mechanism (65) and a water bath device (66), the evaporation tube (62) is obliquely and rotatably installed on a driving shell (111), the distillation flask (61) is sleeved with the oblique lower end of the evaporation tube (62), a first bevel gear (67) is installed on the evaporation tube (62), the oblique upper end of the evaporation tube (62) is rotatably and hermetically connected with the condenser (21), the feeding tube (63) is fixedly connected with the condenser (21), one end of the feeding tube (63) is located at the inner side of the evaporation tube (62), the other end of the feeding tube (63) extends out of the condenser (21), the stirring mechanism (64) comprises a stirring sleeve (641), the stirring sleeve (641) is rotatably installed on the feeding tube (63), an inner magnet (642) is installed on the stirring sleeve (641), and a stirring assembly is installed at the oblique lower end of the stirring sleeve (641), a rotating ring disc (643) is rotatably mounted in the drive shell (111), an outer magnet (644) and a gear ring (645) are mounted on the rotating ring disc (643), and the outer magnet (644) and the inner magnet (642) are coaxially arranged; at least one transmission mechanism (65) is arranged in the driving shell (111), the transmission mechanism (65) comprises a worm (651), a transmission shaft (652), a cylindrical gear (653), a worm wheel (654) and a second bevel gear (655), the worm (651) and the transmission shaft (652) are both rotatably arranged on the driving shell (111), the transmission shaft (652) is provided with the second bevel gear (655) and the worm wheel (654), the worm (651) is meshed with the worm wheel (654) and connected, the cylindrical gear (653) is arranged on the worm (651), the cylindrical gear (653) is meshed with the gear ring (645), and the first bevel gear (67) is meshed with the second bevel gear (655); the water bath device (66) is arranged on the frame (5) and is used for heating the distillation flask (61);

each evaporation mechanism (6) above the evaporation mechanism (6) at the lowest layer is provided with two transmission mechanisms (65), and the adjacent transmission mechanisms (65) of the adjacent evaporation mechanisms (6) are connected through a belt transmission component (68); the driving motor (112) is in transmission connection with one worm (651); the water bath device (66) of the evaporation mechanism (6) at the lowest layer is a heating pot, and the water bath devices (66) of the other evaporation mechanisms (6) are water reservoirs;

circulating water heating mechanism (12) include circulating water pipeline (121), install water pump (122) on circulating water pipeline (121), circulating water pipeline (121) lower extreme and heating pot intercommunication, circulating water pipeline (121) upper end extends to the superiors cistern and installs hard pipe (123), installs flexible outlet pipe (124) on the cistern, hard pipe (123) and flexible outlet pipe (124) lower extreme all install be used for rather than below retort (61) upper surface complex flexible outlet head (125).

6. The drying device for preparing the nano copper oxide-graphite phase carbon nitride composite material according to claim 5, wherein the flexible water outlet pipe (124) is provided with a regulating valve (126), and the hard pipe (123) is provided with a pressure reducing valve (127).

7. The drying device for preparing the nano copper oxide-graphite phase carbon nitride composite material according to claim 5, wherein the second lifting mechanism (4) comprises an electric push rod (41), a guide sleeve (42) and a guide rod (43), the electric push rod (41) and the guide sleeve (42) are installed on the frame (5), the guide rod (43) is slidably installed in the guide sleeve (42), the telescopic end of the electric push rod (41) is connected with the guide rod (43) through a connecting piece (44), a cross rod (45) is fixed on the guide rod (43), and the cross rod (45) is connected with the flexible water outlet pipe (124); the circulating water pipe (121) is installed on the guide bar (43).

8. The drying device for preparing the nano copper oxide-graphite phase carbon nitride composite material according to claim 5, wherein the condenser (21) comprises a condensation shell (211) and a condensation pipe (212), the condensation shell (211) is obliquely installed on the rack (5), guide plates (213) corresponding to the evaporation pipes (62) in a one-to-one mode are fixed on the inner wall of the condensation shell (211), and the guide plates (213) are positioned above the communication position of the evaporation pipes (62) and the condensation shell (211).

9. The drying device for preparing the nano copper oxide-graphite phase carbon nitride composite material according to claim 5, wherein a third bevel gear (113) is further installed on the worm (651) of the evaporation mechanism (6) on the uppermost layer, and a fourth bevel gear (114) meshed and connected with the third bevel gear (113) is installed at the output end of the driving motor (112).

10. The drying device for preparing the nano copper oxide-graphite phase carbon nitride composite material according to claim 5, wherein the stirring assembly comprises an installation seat (646), the installation seat (646) is fixedly connected with the stirring sleeve (641), a plurality of movable blades (647) are hinged on the installation seat (646), and the movable blades (647) are circumferentially distributed along the axis of the stirring sleeve (641).

Technical Field

The invention relates to the technical field of nano composite materials, in particular to a preparation method of a nano copper oxide-graphite phase carbon nitride composite material and a drying device for preparation.

Background

Graphite phase carbon nitride (g-C3N 4) is a slightly water-soluble material with a planar two-dimensional lamellar structure, similar to graphene, and is stacked in a manner that a C-N lamellar structure is taken as a core. g-C3N4 exist in five forms in total, and the carbon nitride of the graphite-like phase at normal temperature is the most stable structure in the five forms. The g-C3N4 has high heat resistance and excellent performance in strong acid and strong alkali resistance. The carbon nitride can be prepared by selecting some nitrogen-rich raw materials to carry out thermal polycondensation. For example: melamine, dicyanodiamine, urea, thiourea, ammonium thiocyanate and the like, and the preparation process is simple and convenient.

The composite material taking g-C3N4 as a matrix gradually shows excellent performance, and the preparation of most of the carbon nitride nano composite materials adopts a common two-step method, namely the preparation of graphite phase carbon nitride and the preparation of the carbon nitride nano composite materials. The two-step synthesis steps and the treatment process are complicated and are not suitable for industrial production. As described in patent application No. 2018113144517 (graphite phase carbon nitride foam composite cuprous oxide quantum dot catalytic material and preparation method thereof), g-C3N4 as a carrier can prepare a high-efficiency hydrogen evolution catalyst. The two-step method is still adopted in the preparation process to prepare the cuprous oxide composite carbon nitride structure, firstly, the preparation of the carbon nitride is carried out, and secondly, the cuprous oxide and the carbon nitride are compounded. As disclosed in patent publication No. CN105032465B (metal oxide/carbon nitride composite material, and method for producing and use thereof), a nanocomposite can be produced by a hydrothermal method after a metal salt is sufficiently mixed with carbon nitride.

In the preparation process, a drying device is required for drying, most of the prior rotary evaporators are used for drying at normal temperature, the rotary evaporators keep flasks filled with reactants and solvents to continuously rotate under the condition of pressure reduction, the bottle walls of the flasks are uniformly heated, and a layer of solution liquid film is attached to the bottle walls of the flasks, so that the evaporation area is increased, the evaporation rate is increased, and the volatile solvents are quickly evaporated.

In the process of vacuumizing the conventional rotary evaporator, because the solvent in the distillation flask is easy to be subjected to bumping or generate large bubbles, the solvent is easy to overflow into the recovery flask after bumping or large bubbles are broken, so that the solvent in the recovery flask is polluted; in addition, the evaporation bottle is heated by a water bath kettle, the evaporation bottle can only be heated from the bottom by the water bath kettle, and the part of the evaporation bottle which rotates to the position above the water surface cannot be continuously heated by water bath in the rotation process of the evaporation bottle, so that the temperature is reduced, and the evaporation speed is influenced; the rotary evaporator is generally only provided with a single distillation flask, has low production efficiency and is not suitable for large-scale batch production.

Disclosure of Invention

The invention aims to solve the problems and designs a preparation method of a nano copper oxide-graphite phase carbon nitride composite material and a drying device for preparation.

The technical scheme of the invention is that the preparation method of the nano copper oxide-graphite phase carbon nitride composite material comprises the following steps:

weighing the first raw material and the second raw material according to the weight ratio of (2-7) to 1, adding the first raw material and the second raw material into a solvent, stirring to uniformly disperse the first raw material and the second raw material in the solvent, and then evaporating and drying through a drying device; wherein the first raw material is melamine or dicyandiamide, and the second raw material is copper nitrate; the usage amount of the first raw material is converted according to the yield of g-C3N4 obtained by calcining the first raw material, wherein the yield is different from 45% to 51% under different calcining conditions;

and grinding the dried solid, putting the ground solid into a container, putting the container into a heating furnace, controlling the temperature at 500-550 ℃, and calcining for 3-5 hours to obtain the nano CuO @ g-C3N4 composite material. The copper oxide can be uniformly distributed on the surface of the carbon nitride, and changes the bright yellow color compared with the pure carbon nitride, and the color is brown.

The solvent is one or more of acetone, ethanol and water.

The container is a quartz ark crucible, and the heating furnace is a tubular heating furnace.

And in the calcining process, nitrogen protection is used, and the airflow speed of the nitrogen protection is 0.4L/min.

The invention also provides a drying device for preparing the nano copper oxide-graphite phase carbon nitride composite material, which comprises a rack, and a rotary evaporation system, a condensation system, a first lifting mechanism and a second lifting mechanism which are arranged on the rack, wherein:

the condensing system comprises a condenser and a collecting bottle, and the lower end of the condenser is sleeved with the collecting bottle;

the rotary evaporation system comprises a rotary driving mechanism, a circulating water heating mechanism and at least two evaporation mechanisms, wherein the rotary driving mechanism comprises a driving shell arranged at the lifting end of the first lifting mechanism, and a driving motor is arranged on the driving shell;

the evaporation mechanism comprises a distillation flask, an evaporation tube, a feeding tube, a stirring mechanism, a transmission mechanism and a water bath device, the evaporation tube is obliquely and rotatably mounted on a driving shell, the distillation flask is connected with the oblique lower end of the evaporation tube in a sleeved mode, a first bevel gear is mounted on the evaporation tube, the oblique upper end of the evaporation tube is rotatably and hermetically connected with a condenser, the feeding tube is fixedly connected with the condenser, one end of the feeding tube is positioned at the inner side of the evaporation tube, the other end of the feeding tube extends out of the condenser, the stirring mechanism comprises a stirring sleeve, the stirring sleeve is rotatably mounted on the feeding tube, an inner magnet is mounted on the stirring sleeve, a stirring assembly is mounted at the oblique lower end of the stirring sleeve, a rotating ring disc is rotatably mounted in the driving shell, an outer magnet and a gear ring are mounted on the rotating ring disc, and the outer magnet and the inner magnet are coaxially arranged; at least one transmission mechanism is arranged in the driving shell and comprises a worm, a transmission shaft, a cylindrical gear, a worm wheel and a second bevel gear, the worm and the transmission shaft are rotatably arranged on the driving shell, the second bevel gear and the worm wheel are arranged on the transmission shaft, the worm is meshed with the worm wheel, the cylindrical gear is arranged on the worm and is meshed with the gear ring, and the first bevel gear is meshed with the second bevel gear; the water bath device is arranged on the frame and used for heating the distillation flask;

each evaporation mechanism above the evaporation mechanism at the lowest layer is provided with two transmission mechanisms, and the adjacent transmission mechanisms of the adjacent evaporation mechanisms are connected through a belt transmission assembly; the driving motor is in transmission connection with one of the worms; the water bath devices of the evaporation mechanisms at the lowest layer are heating pots, and the water bath devices of the other evaporation mechanisms are water reservoirs;

the circulating water heating mechanism comprises a circulating water pipeline, a water pump is mounted on the circulating water pipeline, the lower end of the circulating water pipeline is communicated with the heating pot, the upper end of the circulating water pipeline extends to the reservoir on the uppermost layer and is provided with a hard pipe, a flexible water outlet pipe is mounted on the reservoir, and flexible water outlet heads matched with the upper surface of the distillation flask below the hard pipe and the flexible water outlet pipe are mounted at the lower ends of the hard pipe and the flexible water outlet pipe;

as a further improvement of the invention, the flexible water outlet pipe is provided with an adjusting valve, and the hard pipe is provided with a pressure reducing valve.

As a further improvement of the invention, the second lifting mechanism comprises an electric push rod, a guide sleeve and a guide rod, the electric push rod and the guide sleeve are arranged on the frame, the guide rod is slidably arranged in the guide sleeve, the telescopic end of the electric push rod is connected with the guide rod through a connecting piece, a cross rod is fixed on the guide rod, and the cross rod is connected with the flexible water outlet pipe; the circulating water pipeline is installed on the guide rod.

As a further improvement of the invention, the condenser comprises a condensing shell and a condensing tube, wherein the condensing shell is obliquely arranged on the rack, guide plates which correspond to the evaporating tubes one by one are fixed on the inner wall of the condensing shell, and the guide plates are positioned above the communication position of the evaporating tubes and the condensing shell.

As a further improvement of the invention, a third bevel gear is also arranged on the worm of the evaporation mechanism at the uppermost layer, and a fourth bevel gear which is in meshing connection with the third bevel gear is arranged at the output end of the driving motor.

As a further improvement of the invention, the stirring assembly comprises a mounting seat, the mounting seat is fixedly connected with the stirring sleeve, a plurality of movable blades are hinged on the mounting seat, and the movable blades are circumferentially distributed along the axis of the stirring sleeve.

The invention has the beneficial effects that:

1. the raw materials are wide in source, low in cost and simple and convenient to operate, and the method is suitable for large-scale batch production; the graphite-phase carbon nitride raw material is melamine or dicyandiamide, and the nano CuO @ g-C3N4 composite material can be prepared by a one-step method through calcination;

2. the solvent in the nano composite material prepared by the one-step method can be repeatedly recycled, and no non-solvent is generated;

3. the product obtained by the preparation method has smaller granularity, larger crystal face spacing of the carbon nitride composite material and weaker interlayer bonding force;

4. the drying device adopts a multi-distillation-bottle stacking design, so that the production efficiency is high, and the overall occupied space is small;

5. the stirring assembly can be contacted with the solvent on the upper layer in the distillation flask to prevent the solvent from bumping, when the solvent has larger bubbles, the movable blade can puncture the bubbles to prevent the solvent in the distillation flask from entering the evaporation tube and the collection bottle, and simultaneously, the movable blade rotates at a higher rotating speed to improve the fluidity of the liquid surface air and the evaporation speed;

6. hot water is sprayed to the upper part of the distillation flask through the flexible water outlet head, the defect that only the lower part of the distillation flask is contacted with the hot water is overcome, the whole body of the distillation flask can be contacted with the hot water, the solvent liquid is close to the preset heating temperature to the maximum extent, and the evaporation speed is improved; in addition, because the hot water is continuously contacted with the distillation flask, the drying device can be used at a lower temperature, and the limitation that the conventional rotary evaporator can only be used at normal temperature is overcome.

Drawings

FIG. 1 is an XRD pattern of a nano CuO @ g-C3N4 composite material prepared in example 1 of the present application;

FIG. 2 is a schematic representation of a CuO @ g-C3N4 composite material prepared in example 1 of the present application;

FIG. 3 is a pictorial representation of g-C3N4 material produced in example 1 of the present application;

FIG. 4 is a scanning electron microscope image of the nano CuO @ g-C3N4 composite material prepared in example 1 of the present application;

FIG. 5 is an EDS spectrum of a nano CuO @ g-C3N4 composite prepared in example 1 of the present application;

FIG. 6 is a schematic structural view of example 6;

FIG. 7 is an enlarged view of a portion of FIG. 6 at A;

FIG. 8 is a partial schematic view of the vaporization mechanism of FIG. 6;

in the figure, 1, a rotary evaporation system; 11. a rotation driving mechanism; 111. a drive housing; 112. a drive motor; 113. a third bevel gear; 114. a fourth bevel gear; 12. a circulating water heating mechanism; 121. a circulating water pipeline; 122. a water pump; 123. a rigid tube; 124. a flexible water outlet pipe; 125. a flexible water outlet head; 126. adjusting a valve; 127. a pressure reducing valve; 2. a condensing system; 21. a condenser; 211. a condensing shell; 212. a condenser tube; 213. a baffle; 22. a collection bottle; 3. a first lifting mechanism; 4. a second lifting mechanism; 41. an electric push rod; 42. a guide sleeve; 43. a guide bar; 44. a connecting member; 45. a cross bar; 5. a frame; 6. an evaporation mechanism; 61. a distillation flask; 62. an evaporation tube; 63. a feed pipe; 64. a stirring mechanism; 641. stirring the sleeve; 642. an inner magnet; 643. a rotating ring disc; 644. an outer magnet; 645. a ring gear; 646. a mounting seat; 647. a movable blade; 65. a transmission mechanism; 651. a worm; 652. a drive shaft; 653. a cylindrical gear; 654. a worm gear; 655. a second bevel gear; 66. a water bath device; 67. a first bevel gear; 68. a belt drive assembly.

Detailed Description

In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail below with reference to the accompanying drawings and the detailed description. It should be understood that the detailed description and specific examples, while indicating the scope of the invention, are intended for purposes of illustration only and are not intended to limit the scope of the invention.

It will be understood that when an element is referred to as being "secured to" another element, it can be directly on the other element or intervening elements may also be present. When an element is referred to as being "connected" to another element, it can be directly connected to the other element or intervening elements may also be present. The terms "vertical," "horizontal," "left," "right," and the like as used herein are for illustrative purposes only and do not represent the only embodiments.

Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terminology used herein in the description of the invention is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. As used herein, the term "and/or" includes any and all combinations of one or more of the associated listed items.

The terms "first" and "second" used herein do not denote any particular order or quantity, but rather are used to distinguish one element from another. CuO @ g-C3N4 is a nano copper oxide-graphite phase carbon nitride composite material.

Example 1

In a 100mL round bottom flask 9.804g melamine and 3.038g copper nitrate were weighed, 50mL acetone was added and magnetic stirring was carried out at 25 ℃ for 4h until the copper nitrate was completely dissolved. And a closed system is ensured in the stirring process, and the acetone is prevented from volatilizing.

And (3) evaporating the solvent by using a drying device of a mixed system of copper nitrate and melamine (which is blue-white emulsion at this time), wherein the drying device adopts a rotary evaporator until blue-white powder particles are completely presented in the reaction bottle.

And pouring the powder into a corresponding quartz ark crucible, putting the quartz ark crucible into a heating furnace, raising the temperature to 550 ℃ under the protection of nitrogen at the airflow speed of 0.4L/min, and calcining for 3h to finally obtain a brown product, namely CuO @ g-C3N 4.

The relevant characterization of the product of example 1 is shown in FIGS. 1-4.

Example 2

In a 250mL round bottom flask 19.608g melamine and 3.038g copper nitrate were weighed into 100mL acetone and magnetically stirred at 25 ℃ for 4h until the copper nitrate was completely dissolved.

The copper nitrate and melamine mixed system (now in a blue-white emulsion) was dried using a drying apparatus to evaporate the solvent until the reaction flask was completely filled with blue-white powder particles.

(3) And pouring the powder into a corresponding quartz ark crucible, putting the quartz ark crucible into a heating furnace, raising the temperature to 550 ℃ under the protection of nitrogen at the airflow speed of 0.4L/min, and calcining for 5 hours to obtain a product CuO @ g-C3N 4.

Example 3

In a 100mL round bottom flask, 9.804g of melamine and 3.038g of copper nitrate were weighed, 50mL of a mixture of ethanol and water (ethanol to water volume ratio 7: 3) were added, and magnetic stirring was performed at 25 ℃ for 4h until the copper nitrate was completely dissolved.

The copper nitrate and melamine mixed system (now in a blue-white emulsion) was dried using a drying apparatus to evaporate the solvent until the reaction flask was completely filled with blue-white powder particles.

And pouring the powder into a corresponding quartz ark crucible, putting the quartz ark crucible into a heating furnace, raising the temperature to 550 ℃ under the protection of nitrogen at the airflow speed of 0.4L/min, and calcining for 3 hours to obtain a product CuO @ g-C3N 4.

Example 4

In a 250mL round bottom flask, 11.111g of dicyandiamide and 3.038g of copper nitrate were weighed, 100mL of a mixture of acetone and ethanol (acetone to ethanol volume ratio 7: 3) was added, and magnetic stirring was performed at 25 ℃ for 4h until the copper nitrate was completely dissolved. And a closed system is ensured in the stirring process, and the solvent is prevented from volatilizing.

The copper nitrate and melamine mixed system (now in a blue-white emulsion) was dried using a drying apparatus to evaporate the solvent until the reaction flask was completely filled with blue-white powder particles.

And pouring the powder into a corresponding quartz ark crucible, putting the quartz ark crucible into a heating furnace, raising the temperature to 550 ℃ under the protection of nitrogen at the airflow speed of 0.4L/min, and calcining for 5 hours to obtain a product CuO @ g-C3N 4.

Example 5

In a 100mL round bottom flask, 11.111g of dicyandiamide and 3.038g of copper nitrate were weighed, 50mL of acetone was added, and magnetic stirring was performed at 25 ℃ for 4h until the copper nitrate was completely dissolved. And a closed system is ensured in the stirring process, and the acetone is prevented from volatilizing.

The copper nitrate and melamine mixed system (now in a blue-white emulsion) was dried using a drying apparatus to evaporate the solvent until the reaction flask was completely filled with blue-white powder particles.

And pouring the powder into a corresponding quartz ark crucible, putting the quartz ark crucible into a heating furnace, raising the temperature to 550 ℃ under the protection of nitrogen at the airflow speed of 0.4L/min, and calcining for 3 hours to obtain a product CuO @ g-C3N 4.

Example 6

As shown in fig. 6 to 8, a drying device for preparing a nano copper oxide-graphite phase carbon nitride composite material includes a frame 5, and a rotary evaporation system 1, a condensation system 2, a first lifting mechanism 3 and a second lifting mechanism 4 which are installed on the frame 5, wherein the first lifting mechanism 3 is a lifting column or a lifting platform in the prior art, and wherein:

the condensing system 2 comprises a condenser 21 and a collecting bottle 22, and the lower end of the condenser 21 is sleeved with the collecting bottle 22;

the rotary evaporation system 1 comprises a rotary driving mechanism 11, a circulating water heating mechanism 12 and at least two evaporation mechanisms 6, wherein the rotary driving mechanism 11 comprises a driving shell 111 arranged at the lifting end of the first lifting mechanism 3, and a driving motor 112 is arranged on the driving shell 111;

the evaporation mechanism 6 comprises a distillation flask 61, an evaporation tube 62, a feeding tube 63, a stirring mechanism 64, a transmission mechanism 65 and a water bath device 66, wherein the evaporation tube 62 is obliquely and rotatably arranged on a driving shell 111, the evaporation tube 62 is rotatably arranged on the driving shell 111 through a bearing, the distillation flask 61 is sleeved with the oblique lower end of the evaporation tube 62, a first bevel gear 67 is arranged on the evaporation tube 62, the oblique upper end of the evaporation tube 62 is rotatably and hermetically connected with the condenser 21, a rotary sealing ring is arranged at the joint of the evaporation tube 62 and the condenser 21, the oblique upper end of the evaporation tube 62 is rotatably and hermetically connected with the condenser 21 through the rotary sealing ring, the feeding tube 63 is fixedly connected with the condenser 21, one end of the feeding tube 63 is positioned at the inner side of the evaporation tube 62, the other end of the feeding tube 63 extends out of the condenser 21, and an emptying valve is also arranged at one end of the feeding tube 63 extending out of the condenser 21; the stirring mechanism 64 comprises a stirring sleeve 641, the stirring sleeve 641 is rotatably installed on the feeding pipe 63, an inner magnet 642 is installed on the stirring sleeve 641, specifically, an installation part is arranged on the stirring sleeve 641, a magnetic transmission part is arranged on the evaporation pipe 62, the diameter of the magnetic transmission part is larger than that of other pipe sections, the installation part is located at the magnetic transmission part, a large space is conveniently reserved for arranging the inner magnet 642, meanwhile, the steam can pass through the installation part without blockage, the installation part is rotatably installed on the feeding pipe 63 through a bearing, the inner magnet 642 is installed on the installation part, a stirring assembly is installed at the inclined lower end of the stirring sleeve 641, a rotating ring disk 643 is rotatably installed in the driving shell 111, an outer magnet 644 and a gear ring are installed on the rotating ring disk 643, and the outer magnet 644 and the inner magnet 642 are coaxially arranged; at least one transmission mechanism 65 is arranged in the driving shell 111, the transmission mechanism 65 comprises a worm 651, a transmission shaft 652, a cylindrical gear 653, a worm wheel 654 and a second bevel gear 655, the worm 651 and the transmission shaft 652 are both rotatably arranged on the driving shell 111, the transmission shaft 652 is provided with the second bevel gear 655 and the worm wheel 654, the worm 651 is in meshing connection with the worm wheel 654, the worm 651 is provided with the cylindrical gear 653, the cylindrical gear 653 is in meshing connection with the gear ring 645, and the first bevel gear 67 is in meshing connection with the second bevel gear 655; a water bath device 66 is arranged on the frame 5 for heating the distillation flask 61

Each evaporation mechanism 6 above the evaporation mechanism 6 at the lowest layer is provided with two transmission mechanisms 65, and the adjacent transmission mechanisms 65 of the adjacent evaporation mechanisms 6 are connected through a belt transmission component 68; the driving motor 112 is in transmission connection with one of the worms 651; the water bath device 66 of the evaporation mechanism 6 at the lowest layer is a heating pot, and the water bath devices 66 of the other evaporation mechanisms 6 are water reservoirs;

the circulating water heating mechanism 12 comprises a circulating water pipeline 121, a water pump 122 is installed on the circulating water pipeline 121, the water pump 122 is fixedly installed on the rack 5, the lower end of the circulating water pipeline 121 is communicated with a heating water cavity of a heating pot, namely the lowermost water bath device 66, the upper end of the circulating water pipeline 121 extends to the uppermost reservoir and is provided with a hard pipe 123, a flexible water outlet pipe 124 is installed on the reservoir, and flexible water outlet heads 125 used for being matched with the upper surface of the distillation flask 61 below the hard pipe 123 and the flexible water outlet pipe 124 are installed at the lower ends of the hard pipe 123 and the flexible water outlet pipe 124; the flexible water outlet head 125 is an arc-shaped pipe structure matched with the shape of the upper part of the distillation flask 61, the lower part of the arc-shaped pipe is provided with a water retaining and guiding piece, the water retaining and guiding piece is a cotton sliver, brush hair or sponge, the bottom of the arc-shaped pipe is provided with a water outlet hole, water flows out through the water outlet hole and then contacts with the water retaining and guiding piece, the water retaining and guiding piece can buffer water flow, the impact force of the water is reduced, the water is guided to the distillation flask 61, the water can contact with the upper part of the distillation flask 61 at a lower speed, and the splashing of the water is avoided.

In order to adjust the water outlet speed of the reservoir, an adjusting valve 126 is arranged on the flexible water outlet pipe 124; in order to reduce the impact of water flow when the hard pipe 123 discharges water, a pressure reducing valve 127 is installed on the hard pipe 123.

In order to facilitate the lifting of the driving circulating water pipeline 121 and the flexible water outlet head 125, the second lifting mechanism 4 comprises an electric push rod 41, a guide sleeve 42 and a guide rod 43, the electric push rod 41 and the guide sleeve 42 are installed on the frame 5, the guide rod 43 is slidably installed in the guide sleeve 42, the telescopic end of the electric push rod 41 is connected with the guide rod 43 through a connecting piece 44, a cross rod 45 is fixed on the guide rod 43, and the cross rod 45 is connected with the flexible water outlet pipe 124; circulating water pipeline 121 installs on guide bar 43, and the pipeline section that circulating water pipeline 121 installed on guide bar 43 is the stereoplasm section, can be convenient for install on guide bar 43 along with guide bar 43 goes up and down.

For the steam that produces a plurality of evaporation mechanism 6 condenses, set up condenser 21 and include condensation casing 211 and condenser pipe 212, condensation casing 211 slope is installed on frame 5, be fixed with on the condensation casing 211 inner wall with the guide plate 213 of evaporating pipe 62 one-to-one, guide plate 213 is located evaporating pipe 62 and condensation casing 211's intercommunication department top, condenser pipe 212 is connected with condensate circulating system, condensate circulating system continuously supplies cold water for condenser pipe 212 circulation. By arranging the guide plate 213, the vertically dropped condensate water can be blocked, and the condensate water is prevented from entering the evaporation tube 62 from the communication position of the evaporation tube 62 and the condensation shell 211.

In order to facilitate the driving motor 112 to drive the worm 651 to rotate, the worm 651 of the evaporation mechanism 6 arranged at the uppermost layer is also provided with a third bevel gear 113, and the output end of the driving motor 112 is provided with a fourth bevel gear 114 in meshing connection with the third bevel gear 113.

In order to improve the air fluidity of the liquid surface in the evaporation process, increase the evaporation speed, prevent the solvent from bumping or bubbling and prevent the solvent in the distillation flask 61 from entering the evaporation tube 62 and the collection bottle 22, the stirring assembly comprises an installation seat 646, the installation seat 646 is fixedly connected with a stirring sleeve 641, a plurality of movable blades 647 are hinged on the installation seat 646, and the movable blades 647 are circumferentially distributed along the axis of the stirring sleeve 641. The size of mount pad 646 is less than the bottleneck size of retort 61, and movable vane 647 is folding when accomodating in mount pad 646 inboard, can get into retort 61 by the bottleneck, and when great bubble appears in the solvent, movable vane 647 can pierce the bubble, and movable vane 647 can form one through the rotation and block the barrier, avoids the bubble to break and splashes to evaporating pipe 62 and collecting bottle 22 in.

The working principle of the embodiment is as follows: starting a heating pot, and heating water to a preset temperature by the heating pot; the mixing system of the first raw material, the second raw material and the solvent is placed in a plurality of distillation bottles 61, the movable blades 647 are folded, the length direction of the movable blades 647 is parallel to the axial direction of the stirring sleeve 641, the stirring assembly extends into the distillation bottles 61, the distillation bottles 61 are connected with the evaporation pipe 62 by using bottle clamps, the stirring assembly is not in direct contact with the distillation bottles 61, and the collection bottles 22 are connected with the condensation shell 211 by using the bottle clamps; adjusting the first lifting mechanism 3, wherein the first lifting mechanism 3 drives the rotary driving mechanism 11 and the evaporation mechanism 6 to lift, so that the lower part of the distillation flask 61 is immersed into the water bath device 66;

the driving motor 112 and the water pump 122 are started, the driving motor 112 drives the third bevel gear and the worm 651 of the evaporation mechanism 6 at the uppermost layer to rotate through the fourth bevel gear 114, the worm 651 drives the gear ring 645, the rotating ring disc 643 and the outer magnet 644 to rotate through the cylindrical gear 653, the outer magnet 644 drives the inner magnet 642 at the inner side of the outer magnet 644 to rotate through the magnetic force attracted mutually, further drives the stirring sleeve 641 and the stirring assembly to rotate, the worm 651 drives the worm wheel 654 and the transmission shaft 652 to rotate at a reduced speed, the transmission shaft 652 drives the first bevel gear 67 and the evaporation tube 62 to rotate through the second bevel gear 655, the evaporation tube 62 drives the distillation flask 61 to rotate, the condenser 21 condenses the solvent evaporated from the distillation flask 61, and the collection flask 22 recovers the condensed solvent;

in the rotation process of the stirring sleeve 641, under the action of centripetal force, the movable blades 647 automatically unfold, the solvent is always positioned at the lower part of the distillation flask 61 under the action of self gravity, the movable blades 647 can be rotated to be in contact with the upper layer solvent in the distillation flask 61 to prevent the solvent from bumping, when the solvent has larger bubbles, the movable blades 647 can puncture the bubbles to prevent the solvent in the distillation flask 61 from entering the evaporation tube 62 and the collection bottle 22, and meanwhile, the movable blades 647 rotate at higher rotating speed to improve the fluidity of the liquid surface air and improve the evaporation speed;

the water pump 122 pumps hot water heated to a preset temperature in the heating pot into the hard pipe 123 through the circulating water pipeline 121, the pressure of the hot water is reduced through the pressure reducing valve 127, and the hot water is sprayed onto the distillation bottle 61 on the uppermost layer through the flexible water outlet head 125, so that the defect that only the lower part of the distillation bottle 61 is in contact with the hot water is overcome, the whole body of the distillation bottle 61 can be in contact with the hot water, the solvent liquid is close to the preset heating temperature to the maximum extent, and the evaporation speed is increased; hot water in the water storage tank is discharged through the flexible water outlet pipe 124, the flexible water outlet head 125 sprays the hot water onto the distillation flask 61 below, the flow rate of the discharged water of the flexible water outlet pipe 124 is adjusted to be approximately the same as that of the inlet water by adjusting the adjusting valve 126, the hot water can flow circularly, and the distillation flask 61 can be heated conveniently;

after the solvent is recovered, the driving motor 112, the water pump 122 and the heating pot are closed, the second lifting mechanism 4 is started, the electric push rod 41 drives the guide rod 43 to stably ascend under the guiding action of the guide sleeve 42, the guide rod 43 drives the circulating water pipeline 121, the flexible water outlet pipe 124 and the flexible water outlet head 125 to ascend through the cross rod 45, the hard pipe 123 drives the flexible water outlet head 125 at the uppermost layer to ascend, so that the flexible water outlet head 125 ascends above the distillation flask 61, and the space is opened, so that the distillation flask 61 is convenient to ascend; the first elevating mechanism 3 is then activated, the first elevating mechanism 3 drives the rotary driving mechanism 11 and the evaporating mechanism 6 to ascend, so that the distillation flask 61 is ascended above the water bath device 66, and then the distillation flask 61 can be detached from the evaporating tube 62.

The technical solutions described above only represent the preferred technical solutions of the present invention, and some possible modifications to some parts of the technical solutions by those skilled in the art all represent the principles of the present invention, and fall within the protection scope of the present invention.