双活性基团调控的S型异质结用于增强光催化CO2还原耦合环丙沙星氧化

doi:10.1016/S1872-2067(24)60281-0

催化学报 ›› 2025, Vol. 73: 205-221.DOI: 10.1016/S1872-2067(24)60281-0

双活性基团调控的S型异质结用于增强光催化CO₂还原耦合环丙沙星氧化

李馨悦, 林海莉, 贾雪梅(), 陈士夫, 曹静()

淮北师范大学化学与材料科学学院, 绿色和精准合成化学及应用教育部重点实验室, 安徽省合成化学与应用重点实验室, 安徽淮北 235000

收稿日期:2025-01-02 接受日期:2025-02-10 出版日期:2025-06-18 发布日期:2025-06-12
通讯作者: *电子信箱: XuemeiJia@njust.edu.cn (贾雪梅), caojing@chnu.edu.cn (曹静).
基金资助:
国家自然科学基金(22202077);国家自然科学基金(52272297);安徽省高等学校自然科学研究项目(2024AH030049);安徽省高等学校自然科学研究项目(2024AH040221);安徽省高等学校自然科学研究项目(2023AH050329);安徽省高等学校自然科学研究项目(2022AH010030);安徽省高校(专业)学科带头人培养项目(DTR2023021)

An S-scheme heterojunction engineered with spatially separated dual active groups for simultaneously photocatalytic CO₂ reduction and ciprofloxacin oxidation

Xinyue Li, Haili Lin, Xuemei Jia(), Shifu Chen, Jing Cao()

Key Laboratory of Green and Precise Synthetic and Applications, Ministry of Education; Anhui Provincial Key Laboratory of Synthetic Chemistry and Applications; College of Chemistry and Materials Science, Huaibei Normal University, Huaibei 235000, Anhui, China

Received:2025-01-02 Accepted:2025-02-10 Online:2025-06-18 Published:2025-06-12
Contact: *E-mail: XuemeiJia@njust.edu.cn (X. Jia), caojing@chnu.edu.cn (J. Cao).
Supported by:
National Natural Science Foundation of China(22202077);National Natural Science Foundation of China(52272297);Natural Science Research Project of Anhui Province for Universities(2024AH030049);Natural Science Research Project of Anhui Province for Universities(2024AH040221);Natural Science Research Project of Anhui Province for Universities(2023AH050329);Natural Science Research Project of Anhui Province for Universities(2022AH010030);Anhui Provincial University Discipline (Professional) Leader Cultivation Project(DTR2023021)

摘要/Abstract

摘要：

光催化二氧化碳(CO₂)还原为太阳能燃料是丰富能源供应和减少温室气体排放的有效途径之一. 特别是, 近年来新兴的光催化CO₂还原与有机污染物氧化分解耦合反应体系不仅实现了光生载流子的充分利用, 还达到了能源与环境双赢. 尽管该策略具有广阔的应用前景, 但目前仍面临反应类型有限、目标产物选择性差以及氧化还原反应动力学缓慢等瓶颈问题. 因此, 迫切需要合理设计高效、低成本且具备强氧化还原能力的双功能活性位点催化剂, 以进一步优化整体效率、扩大反应范围, 并深入研究耦合催化反应机理.

为了高效地实现上述耦合反应体系, 本文构建了一种由双活性基团调控的S型异质结(羟基化BiOBr/氨基化g-C₃N₄)光催化剂, 实现了高效的光催化CO₂还原耦合环丙沙星(CIP)氧化反应. 具体而言, 羟基化的BiOBr表面的羟基(OH)基团作为氧化位点, 吸附并活化有机污染物CIP分子; 而氨基功能化的g-C₃N₄中的氨基(NH₂)基团则作为还原位点, 吸附并活化CO₂分子, 从而使光催化氧化还原反应效率最大化. 实验结果表明, 经双活性基团修饰的S型HBOB/ACN异质结表现出显著优于无表面基团调控的S型BOB/CN异质结以及单一活性基团调控的S型HBOB/CN和BOB/ACN异质结的光催化氧化还原性能. 一系列实验和理论计算进一步证实, OH基团和NH₂基团分别负责捕获空穴和电子, 并参与耦合反应体系中CIP的氧化反应以及CO₂的还原反应. 双活性基团的引入不仅有效增强了反应物分子的吸附和活化, 还加快了载流子的分离与迁移, 实现了对载流子的充分利用.

综上所述, 本研究为合理构建具有氧化还原双活性位点的S型异质结, 以实现高效的环境净化与太阳能燃料生成的双功能耦合反应体系, 提供了全新的指导思路.

关键词: 耦合反应体系, S型异质结, 羟基基团, 氨基基团, 双活性位点

Abstract:

Solar-driven CO₂ conversion and pollutant removal with an S-scheme heterojunction provides promising approach to alleviate energy shortage and environmental crisis, yet the comprehensive regulation of the charge separation and the activation sites of reactant molecules remains challenging. Herein, a dual-active groups regulated S-scheme heterojunction for hydroxy-regulated BiOBr modified amino-functionalized g-C₃N₄ (labeled as HBOB/ACN) was designed by spatially separated dual sites with hydroxyl group (OH) and amino group (NH₂) toward simultaneously photocatalytic CO₂ reduction and ciprofloxacin (CIP) oxidation. The optimized HBOB/ACN delivers around 2.74-fold CO yield rate and 1.61-times CIP removal rate in comparison to BiOBr/g-C₃N₄ (BOB/CN) without surface groups, which chiefly ascribed the synergistic effect of OH and NH₂ group. A series of experiments and theoretical calculation unveiled that the OH and NH₂ group trapped holes and electrons to participate in CIP oxidation and CO₂ reduction, respectively. Besides, dual-functional coupled reaction system realized the complete utilization of carriers. This work affords deep insights for dual-group modified S-scheme heterojunctions with redox active sites toward dual-functional coupled reaction system for environment purification and solar fuel production.

Key words: Coupled reaction system, S-scheme heterojunction, Hydroxyl group, Amino group, Dual active sites

李馨悦, 林海莉, 贾雪梅, 陈士夫, 曹静. 双活性基团调控的S型异质结用于增强光催化CO₂还原耦合环丙沙星氧化[J]. 催化学报, 2025, 73: 205-221.

Xinyue Li, Haili Lin, Xuemei Jia, Shifu Chen, Jing Cao. An S-scheme heterojunction engineered with spatially separated dual active groups for simultaneously photocatalytic CO₂ reduction and ciprofloxacin oxidation[J]. Chinese Journal of Catalysis, 2025, 73: 205-221.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(24)60281-0

https://www.cjcatal.com/CN/Y2025/V73/I6/205

图/表 7

Fig. 1. (a) Synthesis procedure of HBOB/ACN heterojunctions. SEM images of HBOB (b), ACN (c) and HBOB/ACN-0.8 (d) composite. HRTEM image (e) and elemental mapping images (f) of HBOB/ACN-0.8 heterojunction.

Fig. 2. XRD patterns (a) and FTIR spectra (b) of the as-synthesized photocatalysts. O 1s (c) and Bi 4f (d) XPS spectra of HBOB and HBOB/ACN-0.8. N 1s (e) and C 1s (f) XPS spectra of ACN and HBOB/ACN-0.8.

Fig. 3. UV-vis diffuse reflectance spectra (a) and the associated band gap energies (b) for the synthesized catalysts. (c) Valence band XPS spectra of BOB, HBOB, CN, and ACN. Theoretical calculations of band structures and density of states for BOB (d), HBOB (e), CN (f) and ACN (g).

Fig. 4. (a, b) Photocatalytic CO2 conversion linked with CIP degradation over the as-prepared photocatalysts. (c) Action spectra of HBOB/ACN-0.8 heterojunction for CO2 conversion coupled with CIP degradation. (d) Photocatalytic redox performance of HBOB/ACN-0.8 heterojunction in different reaction systems. The isotope-labelled 13CO2 test (e), and the recycling (f) of HBOB/ACN-0.8 heterojunction for CO2 conversion coupled with CIP degradation. TPC response (g), PL spectra (h) and TRPL decay curves (i) of BOB, HBOB, CN, ACN and HBOB/ACN-0.8 heterojunction.

Fig. 5. (a) N2 adsorption-desorption isotherms and the homologous pore size distribution plots (inset). The contact angle (b) and CO2 and CIP adsorption energy (c) of BOB, HBOB, CN, ACN and HBOB/ACN-0.8 heterojunction. (d) In situ FTIR spectra of HBOB/ACN-0.8 hybrid. (e) Free energy of CO2 reduction for ACN and HBOB/ACN-0.8 heterojunction.

Fig. 6. AFM height image (a1,b1), surface potential images (a2,b2), and the corresponding line-scanning surface potential profile (a3,b3) of HBOB/ACN-0.8 heterojunction in the dark (a1?a3) and in the light (b1?b3). In situ XPS high-resolution spectra of O 1s (c), Bi 4f (d), and N 1s (e) for HBOB/ACN-0.8 heterojunction.

Fig. 7. Charge density difference (a) and the corresponding side view (b) of HBOB/ACN hybrid. The regions of charge accumulation and depletion were represented by yellow and cyan areas, respectively. Calculated work functions and structural models of BOB (c), HBOB (d), CN (e) and ACN (f). (g) Schematic diagram of HBOB and ACN materials prior to and following contact in the absence of light, and the migration of photo-induced carriers in the HBOB/ACN under light irradiation. (h) The potential reaction mechanisms for CO2 reduction in conjunction with CIP oxidation on the HBOB/ACN-0.8 heterojunction.

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双活性基团调控的S型异质结用于增强光催化CO₂还原耦合环丙沙星氧化

An S-scheme heterojunction engineered with spatially separated dual active groups for simultaneously photocatalytic CO₂ reduction and ciprofloxacin oxidation

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