氮掺杂显著提升BiOBr光催化还原CO2性能研究

doi:10.1016/j.actphy.2025.100055

物理化学学报 >> 2025, Vol. 41 >> Issue (6): 100055.doi: 10.1016/j.actphy.2025.100055

氮掺杂显著提升BiOBr光催化还原CO₂性能研究

宋相海¹^,⁵, 刘晓颖¹, 任智祥¹, 刘想², 汪梅³^,*(), 吴元锋⁴, 周伟强¹, 朱志¹, 霍鹏伟¹^,*()

¹ 江苏大学化学化工学院, 绿色化学与化工技术研究院, 江苏镇江 212013
² 江苏省高职院校绿色能源与低碳材料工程技术研究开发中心, 镇江市高等专科学校, 江苏镇江 212028
³ 江苏大学农业工程学院, 江苏镇江 212013
⁴ 河南工业大学化学化工学院, 河南焦作 454003
⁵ 林产化学与材料国际创新高地, 南京林业大学, 江苏南京 210037

收稿日期:2024-11-26 修回日期:2025-01-23 录用日期:2025-01-23 发布日期:2025-04-19
通讯作者: Email: 1000004927@ujs.edu.cn (汪梅)huopw@ujs.edu.cn (霍鹏伟)
基金资助:
国家自然科学基金(22108102); 国家自然科学基金(22078131); 河南省属高校基本科研业务费专项资金(NSFRF240609); GHfund B(202302026857); 镇江市社会发展指导性科技计划项目(SH2023102); 南京林产化学与材料国际创新高地资助

Insights into the greatly improved catalytic performance of N-doped BiOBr for CO₂ photoreduction

Xianghai Song¹^,⁵, Xiaoying Liu¹, Zhixiang Ren¹, Xiang Liu², Mei Wang³^,*(), Yuanfeng Wu⁴, Weiqiang Zhou¹, Zhi Zhu¹, Pengwei Huo¹^,*()

¹ Institute of Green Chemistry and Chemical Technology, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu Province, China
² Jiangsu Higher Vocational College Engineering Research Center of Green Energy and Low Carbon Materials, Zhenjiang College, Zhenjiang 212028, Jiangsu Province, China
³ School of Agricultural Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu Province, China
⁴ School of Chemistry and Chemical Engineering, Henan Polytechnic University, Jiaozuo 454003, Henan Province, China
⁵ International Innovation Center for Forest Chemicals and Materials, Nanjing Forestry University, Nanjing 210037, Jiangsu Province, China

Received:2024-11-26 Revised:2025-01-23 Accepted:2025-01-23 Published:2025-04-19
Contact: Email: 1000004927@ujs.edu.cn (Mei Wang)huopw@ujs.edu.cn (Pengwei Huo)
Supported by:
the National Natural Science Foundation of China(22108102); the National Natural Science Foundation of China(22078131); the Fundamental Research Funds for the Universities of Henan Province(NSFRF240609); the GHfund B(202302026857); the Science and Technology Planning Social Development Project of Zhenjiang City(SH2023102); the International Innovation Center for Forest Chemicals and Materials of Nanjing Forestry

摘要/Abstract

摘要：

光催化还原二氧化碳(CO₂)是一种有望解决全球能源与环境问题的方法。寻找在CO₂转化方面具有高活性和高选择性的催化剂受到了广泛关注。本研究采用简单的水热法合成了超薄氮掺杂的BiOBr纳米片。系统的实验结果表明，氮掺杂降低了BiOBr纳米片的厚度并增加了其比表面积。此外，光生载流子迁移效率和CO₂吸附能力显著增强，从而提高了光催化还原CO₂性能。实验结果表明，2N-BiOBr具有最佳的催化性能，反应在水中进行时，CO的生成速率为18.28 μmol·g⁻¹·h⁻¹，是纯BiOBr的三倍，且CO选择性接近100%。利用原位FTIR和DFT模拟研究了潜在的光催化机制。机理研究表明，氮原子取代氧原子作为吸附中心时，相比于O―H，BiOBr对CO₂的吸附选择性显著增强，并促进了关键反应中间体的形成。本研究为高效光催化材料的制备与开发提供了新的视角，并为光催化技术在能源与环境科学中的应用提供了理论支持。

关键词: N掺杂, CO₂吸附, 超薄BiOBr, 光催化剂, CO₂还原

Abstract:

Photocatalytic carbon dioxide (CO₂) reduction represents a hopeful approach to addressing global energy and environmental issues. The quest for catalysts that demonstrate both high activity and selectivity for CO₂ conversion has attracted significant attention. In this study, ultrathin N-doped BiOBr was synthesized using a simple straightforward method. Systematic experimental results indicated that N-doping reduced the thickness of the BiOBr nanosheets and increased their specific surface area. Moreover, the efficiency of photogenerated charge carrier migration and the CO₂ adsorption capacity were significantly enhanced, contributing to improved CO₂ photoreduction performance. Experimental results showed that the 2N-BiOBr exhibited the best catalytic performance, with a CO evolution rate of 18.28 μmol·g⁻¹·h⁻¹ and nearly 100% CO selectivity in water, which was three times higher than that of pure BiOBr. The potential photocatalytic mechanism was investigated using in situ FTIR analysis and DFT simulations. Mechanistic studies revealed that N atoms replaced O atoms as adsorption centers, enhancing the strong adsorption selectivity towards CO₂ over O―H in BiOBr and facilitating the formation of key reaction intermediates. This study provides new perspectives on the creation and development of effective photocatalytic materials, offering theoretical support for the application of photocatalytic technology in energy and environmental science.

Key words: N-doping, CO₂ adsorption, Ultrathin BiOBr, Photocatalyst, CO₂ reduction

宋相海, 刘晓颖, 任智祥, 刘想, 汪梅, 吴元锋, 周伟强, 朱志, 霍鹏伟. 氮掺杂显著提升BiOBr光催化还原CO₂性能研究[J]. 物理化学学报, 2025, 41(6), 100055. doi: 10.1016/j.actphy.2025.100055

Xianghai Song, Xiaoying Liu, Zhixiang Ren, Xiang Liu, Mei Wang, Yuanfeng Wu, Weiqiang Zhou, Zhi Zhu, Pengwei Huo. Insights into the greatly improved catalytic performance of N-doped BiOBr for CO₂ photoreduction[J]. Acta Phys. -Chim. Sin. 2025, 41(6), 100055. doi: 10.1016/j.actphy.2025.100055

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100055

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I6/100055

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Sample	Specific surface area (m²·g⁻¹)	Pore volume (cm³·g⁻¹)	Average pore diameter (nm)
BiOBr	2.95	0.01	10.01
2N-BiOBr	6.45	0.04	30.38

Catalysts	τ₁ (ns)	τ₂ (ns)	B₁	B₂	τ_av (ns) ^a
BiOBr	16.36	126.15	3164.14	256.72	58.61
2N-BiOBr	18.84	169.59	2955.06	183.35	72.86

catalyst	Sacrificial agent	CO evolution (μmol·g⁻¹·h⁻¹)	Ref.
2N-BiOBr	−	18.28	This work
Vo-R Bi₂₄O₃₁Br₁₀	−	14.80	[43]
BiOBr-4	−	4.45	[46]
NH₂-MIL- 53(Fe)	TEOA	17.52	[63]
Ce/ZnFe₂O₄	−	1.7	[64]
SnFe₂O₄/α- Fe₂O₃	−	2.87	[65]
ZnIN₂S₄/BiVO₄	−	4.75	[66]
P/Bi-BOB-0.25	−	3.1	[67]
Co-BiOBr-0.5	−	11.71	[68]
BSB-16	−	7.4	[69]
BiOBr_0.6Cl_0.4	−	15.86	[70]

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氮掺杂显著提升BiOBr光催化还原CO₂性能研究

Insights into the greatly improved catalytic performance of N-doped BiOBr for CO₂ photoreduction

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