B修饰g-C3N4的制备及其光催化CO2还原

何醒丽; 孙满营; 苏通明

doi:10.12434/j.issn.2097-2547.20240415

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B修饰g-C₃N₄的制备及其光催化CO₂还原

二氧化碳催化转化与资源化利用 | 更新时间：2025-05-29

- B修饰g-C₃N₄的制备及其光催化CO₂还原
- Preparation of B modified g-C₃N₄ and their photocatalytic CO₂ reduction
- 低碳化学与化工 2025, 50(5): 18-31.
- 作者机构：
  
  广西大学化学化工学院广西电化学能源材料重点实验室，广西南宁 530004
- 作者简介：
  
  何醒丽（2000—），硕士研究生，研究方向为光催化CO2还原，E-mail：hexinglihxl@163.com。
  苏通明（1988—），博士，副教授，研究方向为光催化表界面工程，E-mail：sutm@gxu.edu.cn。
- 基金信息：
  
  国家自然科学基金(22208065);广西自然科学基金(2022GXNSFBA035483)
- DOI：10.12434/j.issn.2097-2547.20240415
  中图分类号： TQ034;O643.36
- 收稿日期：2024-10-09，
  
  修回日期：2024-11-01，
  
  纸质出版日期：2025-05-25
- 稿件说明：
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何醒丽,孙满营,苏通明.B修饰g-C₃N₄的制备及其光催化CO₂还原[J].低碳化学与化工,2025,50(05):18-31.

HE Xingli,SUN Manying,SU Tongming.Preparation of B modified g-C₃N₄ and their photocatalytic CO₂ reduction[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(05):18-31.
何醒丽,孙满营,苏通明.B修饰g-C₃N₄的制备及其光催化CO₂还原[J].低碳化学与化工,2025,50(05):18-31. DOI： 10.12434/j.issn.2097-2547.20240415.

HE Xingli,SUN Manying,SU Tongming.Preparation of B modified g-C₃N₄ and their photocatalytic CO₂ reduction[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(05):18-31. DOI： 10.12434/j.issn.2097-2547.20240415.

摘要

石墨氮化碳（g-C

）是光催化CO

还原的理想催化剂之一，然而光生载流子的快速复合限制了g-C

的应用。采用水热法处理由三聚氰胺和B

组成的混合物，然后焙烧水热反应产物，制备了一系列B修饰g-C

（

-B-HCN，

为B

与三聚氰胺的物质的量之比）。采用XRD和FT-IR等对

-B-HCN的晶体结构和官能团等进行了表征，并研究了

-B-HCN的光催化CO

还原制CO性能和相应反应机理。结果表明，

-B-HCN具有较大的比表面积（11.8~24.6 m

/g），因此表现出较强的CO

吸附性能。在使用了400 nm截止滤光片的300 W氙灯照射下反应5 h，0.20-B-HCN表现出最优的催化性能，其CO生成速率为6.88 μmol/(g·h)，分别是一步焙烧法制得的g-C

（1.24 μmol/(g·h)）和未经B修饰的HCN-1（1.73 μmol/(g·h)）的5.54倍和3.97倍。在相同条件下第3次循环中光照5 h时，0.20-B-HCN的CO生成速率为6.53 μmol/(g·h)，表明0.20-B-HCN具有良好的稳定性。

-B-HCN光催化CO

还原为CO的路径为：CO

→ COOH* → CO* → CO。

Abstract

Graphitic carbon nitride (g-C

) is one of the ideal catalysts for photocatalytic CO

reduction. However

the application of g-C

is limited due to the rapid recombination of photogenerated carriers. The mixture of melamine and B

was treated by hydrothermal method

and then a series of B-modified g-C

(

-B-HCN

is the molar ratio of B

and melamine) was prepared by cal

cining the hydrothermal reaction product. The crystal structures and functional groups of

-B-HCN were characterized by XRD and FT-IR

etc. And the photocatalytic performance and corresponding reaction mechanism of

-B-HCN for CO

reduction to CO were studied. The results show that

-B-HCN has large specific surface area (11.8 m

/g to 24.6 m

/g)

thus exhibiting strong CO

adsorption performances. Under irradiation by 300 W xenon lamp with 400 nm cut-off filter for 5 h

0.20-B-HCN exhibits the best photocatalytic performance with CO generation rate of 6.88 μmol/(g·h)

which is 5.54 times greater than that of g-C

(1.24 μmol/(g·h)) obtained by one-step calcination method and 3.97 times greater than that of HCN-1 (1.73 μmol/(g·h)) without B modification. Irradiation for 5 h in the third cycle under the same conditions

the CO generation rate of 0.20-B-HCN is 6.53 μmol/(g·h)

which indicates that 0.20-B-HCN has fairly high stability. The pathway of photocatalytic CO

reduction to CO by

-B-HCN is as follows: CO

→ COOH* → CO* → CO.

关键词

Keywords

references

ISMAEL M . Environmental remediation and sustainable energy generation via photocatalytic technology using rare earth metals modified g-C 3 N 4 : A review [J ] . Journal of Alloys and Compounds , 2023 , 931 : 167469 .

PAN Q S , WU Y F , SU X X , et al . A review on the recent development of bismuth-based catalysts for CO 2 photoreduction [J ] . Journal of Molecular Structure , 2023 , 1294 : 136404 .

LI Y R , LI S T , HUANG H W . Metal-enhanced strategies for photocatalytic and photoelectrochemical CO 2 reduction [J ] . Chemical Engineering Journal , 2023 , 457 : 141179 .

赵梦迪 , 李永利 , 王金淑 . g-C 3 N 4 材料在光催化能源转换领域的新进展 [J ] . 工程科学学报 , 2022 , 44 ( 4 ): 641 - 653 .

ZHAO M D , LI Y L , WANG J S . Recent progress of graphitic phase carbon nitride photocatalytic materials on solar energy conversion [J ] . Chinese Journal of Engineering , 2022 , 44 ( 4 ): 641 - 653 .

GUO R T , XIA C , BI Z X , et al . Recent progress of photothermal effect on photocatalytic reduction of CO 2 [J ] . Fuel Processing Technology , 2023 , 241 : 107617 .

LI Z H , HAN B C , BAI W C , et al . Photocatalytic CO 2 RR for gas fuel production: Opportunities and challenges [J ] . Separation and Purification Technology , 2023 , 324 : 124528 .

XU H Y , WANG Z L , LIAO H H , et al . Proximity of defects and Ti-H on hydrogenated SrTiO 3 mediated photocatalytic reduction of CO 2 to C 2 H 2 [J ] . Applied Catalysis B: Environmental , 2023 , 336 : 122935 .

薛义松 , 郭恩言 , 卢启芳 . Bi 2 MoO 6 /Ni 3 V 2 O 8 异质结构纳米纤维的合成及光催化性能研究 [J ] . 聊城大学学报（自然科学版） , 2022 , 35 ( 6 ): 58 - 67 .

XUE Y S , GUO E Y , LU Q F . Study on preparation and photocatalytic properties of Bi 2 MoO 6 /Ni 3 V 2 O 8 heterostructured nanofibers [J ] . Journal of Liaocheng University (Natural Science Edition) , 2022 , 35 ( 6 ): 58 - 67 .

YANG X , CHENG J , YANG X , et al . MOF-derived Cu@Cu 2 O heterogeneous electrocatalyst with moderate intermediates adsorption for highly selective reduction of CO 2 to methanol [J ] . Chemical Engineering Journal , 2022 , 431 : 134171 .

TIAN T , JIN X Y , GUO N , et al . CdS/ethylenediamine nanowires 3D photocatalyst with rich sulfur vacancies for efficient syngas production from CO 2 photoreduction [J ] . Applied Catalysis B: Environmental , 2022 , 308 : 121227 .

HU Q , CHEN L Y , XIE X L , et al . Construction of electron bridge and activation of MoS 2 inert basal planes by Ni doping for enhancing photocatalytic hydrogen evolution [J ] . Acta Physico Chimica Sinica , 2024 , 40 ( 11 ): 2406024 .

ZHANG T X , MENG F L , GAO M M , et al . Porous host-guest MOF-semiconductor hybrid with multisites heterojunctions and modulable electronic band for selective photocatalytic CO 2 conversion and H 2 evolution [J ] . Small , 2023 , 19 ( 39 ): 2301121 .

LIU Y H , WANG Y , SHANG J , et al . Construction of a novel m etal-free heterostructure photocatalyst PRGO/TP-COF for enhanced photocatalytic CO 2 reduction [J ] . Applied Catalysis B: Environment and Energy , 2024 , 350 : 123937 .

OMR H A E , PUTIKAM R , FENG S P , et al . Synergistic role of Cu—C and Cu—N dual bonding of nanostructured g-C 3 N 4 /Cu 2 SnS 3 photocatalysts for efficient CO 2 conversion to CO [J ] . Applied Catalysis B: Environmental , 2023 , 339 : 123103 .

LI J Y , WANG X H , HUANG L , et al . Ultrathin mesoporous graphitic carbon nitride nanosheets with functional cyano group decoration and nitrogen-vacancy defects for an efficient selective CO 2 photoreduction [J ] . Nanoscale , 2021 , 13 ( 29 ): 12634 - 12641 .

CUI L F , SONG J L , MCGUIRE A F , et al . Constructing highly uniform onion-ring-like graphitic carbon nitride for efficient visible-light-driven photocatalytic hydrogen evolution [J ] . ACS Nano , 2018 , 12 ( 6 ): 5551 - 5558 .

WANG Z Y , CHEN M J , HUANG Y , et al . Self-assembly synthesis of boron-doped graphitic carbon nitride hollow tubes for enhanced photocatalytic NO x removal under visible light [J ] . Applied Catalysis B: Environmental , 2018 , 239 : 352 - 361 .

WANG W K , ZHOU H J , LIU Y Y , et al . Formation of B-N-C coordination to stabilize the exposed active nitrogen atoms in g-C 3 N 4 for dramatically enhanced photocatalytic ammonia synthesis performance [J ] . Small , 2020 , 16 ( 13 ): 1906880 .

CHEN Y L , YU M F , HUANG G C , et al . Interlayer charge transfer over graphitized carbon nitride enabling highly-efficient photocatalytic nitrogen fixation [J ] . Small , 2022 , 18 ( 52 ): 2205388 .

李星杰 , 孙玮 , 明邱焱 , 等 . 硫掺杂g-C 3 N 4 制备及其光催化产氢性能研究 [J ] . 聊城大学学报（自然科学版） , 2024 , 37 ( 1 ): 70 - 75 .

LI X J , SUN W , MING Q Y , et al . Preparation of sulfur-doped g-C 3 N 4 and its photocatalytic performance for hydrogen evolution [J ] . Journal of Liaocheng University (Natural Science Edition) , 2024 , 37 ( 1 ): 70 - 75 .

LU W Y , QI L Y , DONG D C , et al . A comparison study of photocatalytic performance of g-C 3 N 4 prepared from different precursors for the activation of different peroxides [J ] . Separation and Purification Technology , 2023 , 327 : 124904 .

LIU J H , ZHANG T K , WANG Z C , et al . Simple pyrolysis of urea into graphitic carbon nitride with recyclable adsorption and photocatalytic activity [J ] . Journal of Materials Chemistry , 2011 , 21 ( 38 ): 14398 .

WANG Y , LI H R , YAO J , et al . Synthesis of boron doped polymeric carbon nitride solids and their use as metal-free catalysts for aliphatic C—H bond oxidation [J ] . Chemical Science , 2011 , 2 ( 3 ): 446 - 450 .

VEISI P , SEYED D , MIR S . Effect of contact interface type in charge transfer mechanism and visible-light photocatalytic activity of ZnO-g-C 3 N 4 heterostructures [J ] . Materials Research Bulletin , 2023 , 167 : 112428 .

AKHTAR T , NASIR H , SITARA E , et al . Fabrication of novel Ag nanoparticles decorated ZrO 2 /g-C 3 N 4 ternary heterojunction interface for photocatalytic reduction of nitroaromatic compounds [J ] . Surfaces and Interfaces , 2023 , 39 : 102997 .

DONG H , GUO X T , YANG C , et al . Synthesis of g-C 3 N 4 by different precursors under burning explosion effect and its photocatalytic degradation for tylosin [J ] . Applied Catalysis B: Environmental , 2018 , 230 : 65 - 76 .

LAN Z A , ZHANG G G , WANG X C . A facile synthesis of Br-modified g-C 3 N 4 semiconductors for photoredox water splitting [J ] . Applied Catalysis B: Environmental , 2016 , 192 : 116 - 125 .

SING K S W . Reporting physisorption data for gassolid systems with special reference to the determination of surface area and porosity (Recommendations 1984) [J ] . 1985 , 57 ( 4 ): 603 - 619 .

MOHAMED M A , ZAIN M F , JEFFERY L , et al . Constructing bio-templated 3D porous microtubular C-doped g-C 3 N 4 with tunable band structure and enhanced charge carrier separation [J ] . Applied Catalysis B: Environmental , 2018 , 236 : 265 - 279 .

GAO M M , LI Z Y , SU X J , et al . 2D/2D MgO/g-C 3 N 4 S-scheme heterogeneous tight with Mg—N bonds for efficient photo-Fenton degradation: Enhancing both oxygen vacancy and charge migration [J ] . Chemosphere , 2023 , 343 : 140285 .

CHEN P F , XING P X , CHEN Z Q , et al . Rapid and energy-efficient preparation of boron doped g-C 3 N 4 with excellent performance in photocatalytic H 2 -evolution [J ] . International Journal of Hydrogen Energy , 2018 , 43 ( 43 ): 19984 - 19989 .

HARIKRISHNAN L , RAJARAM M , NATARAJAN A , et al . Boron-doped exfoliated g-C 3 N 4 nanosheet-based phosphors for white light-emission and photocatalytic degradation [J ] . ACS Applied Nano Materials , 2023 , 6 ( 18 ): 16947 - 16959 .

WANG R N , WANG Z , QIU Z Y , et al . Nanoscale 2D g-C 3 N 4 decorating 3D hierarchical architecture LDH for artificial photosynthesis and mechanism insight [J ] . Chemical Engineering Journal , 2022 , 448 : 137338 .

LIU Y Z , ZHAO L , ZENG X H , et al . Efficient photocatalytic reduction of CO 2 by improving adsorption activation and carrier utilization rate through N-vacancy g-C 3 N 4 hollow microtubule [J ] . Materials Today Energy , 2023 , 31 : 101211 .

SONG X H , ZHANG X Y , LI X , et al . Enhanced light utilization efficiency and fast charge transfer for excellent CO 2 photoreduction activity by constructing defect structures in carbon nitride [J ] . Journal of Colloid and Interface Science , 2020 , 578 : 574 - 583 .

FANG R M , YANG Z Q , KADIROVA Z C , et al . High-efficiency photoreduction of CO 2 to solar fuel on alkali intercalated ultra-thin g-C 3 N 4 nanosheets and enhancement mechanism investigation [J ] . Applied Surface Science , 2022 , 598 : 153848 .

OJHA N , BAJPAI A , KUMAR S . Visible light-driven enhanced CO 2 reduction by water over Cu modified S-doped g-C 3 N 4 [J ] . Catalysis Science & Technology , 2019 , 9 ( 17 ): 4598 - 4613 .

RAN L , LI Z W , RAN B , et al . Engineering single-atom active sites on covalent organic frameworks for boosting CO 2 photoreduction [J ] . Journal of the American Chemical Society , 2022 , 144 ( 37 ): 17097 - 17109 .

CHEN F F , CHEN J B , LI L Y , et al . g-C 3 N 4 microtubes@CoNiO 2 nanosheets P-N heterojunction with a hierarchical hollow structure for efficient photocatalytic CO 2 reduction [J ] . Applied Surface Science , 2022 , 579 : 151997 .

QIN H , GUO R T , LIU X Y , et al . 0D NiS 2 quantum dots modified 2D g-C 3 N 4 for efficient photocatalytic CO 2 reduction [J ] . Colloids and Surfaces A: Physicochemical and Engineering Aspects , 2020 , 600 : 124912 .

HE W J , WEI Y C , XIONG J , et al . Boosting selective photocatalytic CO 2 reduction to CO over dual-core@shell structured Bi 2 O 3 /Bi 2 WO 6 @g-C 3 N 4 catalysts with strong interaction interface [J ] . Separation and Purification Technology , 2022 , 300 : 121850 .

LI Q , SUN Z X , WANG H Q , et al . Insight into the enhanced CO 2 photocatalytic reduction performance over hollow-structured Bi-decorated g-C 3 N 4 nanohybrid under visible-lig ht irradiation [J ] . Journal of CO 2 Utilization , 2018 , 28 : 126 - 136 .

XIAO Y , MEN C Z , CHU B X , et al . Spontaneous reduction of copper on Ti 3 C 2 T x as fast electron transport channels and active sites for enhanced photocatalytic CO 2 reduction [J ] . Chemical Engineering Journal , 2022 , 446 : 137028 .

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