二维银修饰氮化碳/一维二乙烯三胺改性硫化镉S-型异质结及其高效光催化产过氧化氢性能

doi:10.1016/S1872-2067(26)65174-1

催化学报 ›› 2026, Vol. 90: 231-242.DOI: 10.1016/S1872-2067(26)65174-1

二维银修饰氮化碳/一维二乙烯三胺改性硫化镉S-型异质结及其高效光催化产过氧化氢性能

陈浩然^a, 傅俊伟^b, Graham Dawson^c, 张金锋^a^,^*(), 彭青坡^a^,^*(), 代凯^a^,^*()

^a 淮北师范大学化学与化工学院, 淮北市小分子资源低碳转化重点实验室, 安徽省污染物敏感材料与环境修复重点实验室, 绿色和精准合成化学及应用教育部重点实验室, 安徽淮北 235000
^b 中南大学物理学院, 湖南长沙 410083
^c 西安交通利物浦大学化学与材料科学系, 江苏苏州 215123

收稿日期:2026-02-21 接受日期:2026-03-24 出版日期:2026-11-18 发布日期:2026-09-09
通讯作者: *电子信箱: daikai940@chnu.edu.cn (代凯),
jfzhang@chnu.edu.cn (张金锋),
pengqingpo@chnu.edu.cn (彭青坡).
基金资助:
国家自然科学基金(22578154);国家自然科学基金(22278169);安徽省高校优秀青年骨干人才访学研究计划(gxgnfx2021119);安徽省学科专业领军人才培育项目(DTR2024015)

2D Ag modified g-C₃N₄/1D CdS-diethylenetriamine S-scheme heterojunction with enhanced photocatalytic H₂O₂ production

Haoran Chen^a, Junwei Fu^b, Graham Dawson^c, Jinfeng Zhang^a^,^*(), Qingpo Peng^a^,^*(), Kai Dai^a^,^*()

^a Key Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, Anhui Province Key Laboratory of Pollutant Sensitive Materials and Environmental Remediation, Huaibei Key Laboratory for Low-Carbon Conversion of Small-Molecule Resources, School of Chemistry and Chemical Engineering, Huaibei Normal University, Huaibei 235000, Anhui, China
^b School of Physics, Central South University, Changsha 410083, Hunan, China
^c Department of Chemistry and Materials Science, Xi’an Jiaotong Liverpool University, Suzhou 215123, Jiangsu, China

Received:2026-02-21 Accepted:2026-03-24 Online:2026-11-18 Published:2026-09-09
Contact: *E-mail:daikai940@chnu.edu.cn(K. Dai),jfzhang@chnu.edu.cn(J. Zhang),pengqingpo@chnu.edu.cn(Q. Peng).
Supported by:
National Natural Science Foundation of China(22578154);National Natural Science Foundation of China(22278169);Visiting Scholar Research Program for Outstanding Young Backbone Talents of Anhui Province Universities(gxgnfx2021119);Anhui Province Discipline (specialty) Professional Leader Cultivation Project(DTR2024015)

摘要/Abstract

摘要：

过氧化氢(H₂O₂)是绿色氧化剂与新型能源载体, 传统蒽醌法生产工艺能耗高、污染大, 而光催化产过氧化氢(PHP)符合绿色可持续发展理念, 成为研究热点. 单一半导体光催化剂普遍存在光吸收范围窄、载流子复合严重、活性位点不足等问题, 严重限制产率提升. 石墨相氮化碳(g-C₃N₄)因稳定性好、成本低备受关注, 但纯g-C₃N₄光生电子-空穴对易复合, 催化效率有限. 构建S-型异质结可高效分离载流子并保留强氧化还原能力, 结合贵金属修饰与形貌调控, 是实现高效PHP的关键策略. 本研究旨在设计并构建高性能S-型异质结光催化剂, 为高效、绿色光催化制备H₂O₂提供新思路与实验支撑.

本文采用浸渍热解法制备银修饰氮化碳(Ag-PCN), 再通过一步水热法将其与二乙烯三胺改性硫化镉(CdS-D)复合, 成功构建10% Ag-PCN/CdS-D 1D/2D S型异质结. X-射线衍射、红外光谱(FT-IR)、X-射线光电子能谱等表征证实Ag、C、N、Cd、S元素均匀分布, Ag以金属态成功掺杂, CdS-D以纳米棒形式原位生长在Ag-PCN纳米片上, 形成紧密接触的异质结构. 比表面积测试结果显示, 复合材料比表面积达107.42 m² g^-1, 高于纯样, 可提供更多活性位点. 紫外-可见光漫反射光谱、瞬态光电流与电化学抗阻谱测试表明, Ag掺杂拓宽可见光吸收范围, S-型异质结显著降低电荷转移电阻, 提升载流子分离与迁移效率. 性能测试显示, 10% Ag-PCN/CdS-D在纯水中H₂O₂产率高达3128 μmol g^-1 h^-1, 分别是纯PCN (35.64 μmol g^-1 h^-1)、Ag-PCN(87.54 μmol g^-1 h^-1)和CdS-D (2398 μmol g^-1 h^-1)的87.8、35.7和1.3倍, 且稳定性优异. 自由基捕获、电子顺磁共振与原位FT-IR证实, •O₂^-为关键中间体, 反应遵循2e^-氧还原路径. 密度泛函理论计算表明, Ag降低Ag-PCN功函数, S-型异质结可构建强内建电场, 实现低活性载流子界面复合, 保留高活性载流子参与反应, 从而大幅提升光催化性能.

综上, 本研究成功开发10% Ag-PCN/CdS-D S型异质结光催化剂, 揭示其载流子分离机制与构效关系, 为高效光催化产过氧化氢体系的设计提供实验与理论支撑, 有望推动绿色氧化技术与清洁能源转化领域的发展.

关键词: 光催化H₂O₂生产, S型异质结, 银修饰氮化碳, 二乙烯三胺改性硫化镉

Abstract:

Photocatalytic hydrogen peroxide (H₂O₂) production has emerged as an optimized pathway for sustainable energy conversion and environmental remediation. However, the severe carrier recombination in single semiconductors significantly restricts its efficiency. To resolve this issue, Ag-modified g-C₃N₄ (Ag-PCN) was prepared via an impregnation-pyrolysis method, and the Ag-PCN/CdS-diethylenetriamine (Ag-PCN/CdS-D) S-scheme heterojunction was further constructed with CdS-D through a hydrothermal route, which effectively enhanced the photocatalytic H₂O₂ production (PHP) activity. This improvement is attributed to the fact that the introduction of Ag nanoparticles and diethylenetriamine not only optimizes visible light absorption but plays a crucial role in regulating the band structure and facilitating charge transfer. Furthermore, the 1D nanorods are anchored onto the 2D nanosheets to form a heterostructure. Such a unique S-scheme heterojunction enables efficient carrier separation at the PCN/CdS interface, resulting in a significant improvement in the PHP performance. Finally, the optimized Ag-PCN/CdS-D heterojunction exhibited an H₂O₂ yield of 3128 μmol g^-1 h^-1 in pure water, which was higher than those of pure PCN (35.64 μmol g^-1 h^-1) and CdS-D (2398 μmol g^-1 h^-1). This work lays the groundwork for the rational design of and construction of high-performance photocatalysts for H₂O₂ production.

Key words: Photocatalytic H₂O₂ production, S-scheme heterojunction, Ag-modified g-C₃N₄, CdS-diethylenetriamine

陈浩然, 傅俊伟, Graham Dawson, 张金锋, 彭青坡, 代凯. 二维银修饰氮化碳/一维二乙烯三胺改性硫化镉S-型异质结及其高效光催化产过氧化氢性能[J]. 催化学报, 2026, 90: 231-242.

Haoran Chen, Junwei Fu, Graham Dawson, Jinfeng Zhang, Qingpo Peng, Kai Dai. 2D Ag modified g-C₃N₄/1D CdS-diethylenetriamine S-scheme heterojunction with enhanced photocatalytic H₂O₂ production[J]. Chinese Journal of Catalysis, 2026, 90: 231-242.

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https://www.cjcatal.com/CN/Y2026/V90/I11/231

图/表 6

Fig. 1. Schematic illustration of the synthetic route for 10%Ag-PCN/CdS-D.

Fig. 2. (a) XRD pattern of PCN, Ag-PCN, 10%Ag-PCN/CdS-D, and CdS-D. (b) FT-IR spectra of Ag-PCN and the 10%Ag-PCN/CdS-D. (c) Photoluminescence spectra of samples. (d-g) SEM images of PCN, Ag-PCN, CdS-D, 10%Ag-PCN/CdS-D. TEM (h) and HRTEM (i) images of 10%Ag-PCN/CdS-D. (j) Elemental mapping of 10%Ag-PCN/CdS-D.

Fig. 3. (a) The XPS spectra of pristine Ag-PCN, 10%Ag-PCN/CdS-D, and CdS-D. The survey XPS spectra: (b) Cd 3d, (c) C 1s, (d) S 2p, (e) N 1s, (f) Ag 3d.

Fig. 4. (a) N2 adsorption-desorption isotherms of the prepared samples. (b) SBET of PCN, Ag-PCN, 10%Ag-PCN/CdS-D, and CdS-D. UV-vis DRS (c) and corresponding profiles (d) derived from the transformed Kubelka-Munk model as a function of incident photon energy for the as-fabricated specimens. (e) Mott-Schottky plots for CdS-D. (f) Mott-Schottky plots for Ag-PCN. (g) The band structure of Ag-PCN and CdS-D. (h) Photocurrent-time curves of photocatalysts. (i) Nyquist plots of electrochemical impedance spectra.

Fig. 5. (a) The catalytic PHP performance graph. (b) The productions of H2O2 with prolonged reaction time. (c) Comparison of H2O2 production by 10%Ag-PCN/CdS-D under different conditions over 1 h: H2O, EDTA (0.5 mmol L-1), NBT (0.06 mmol L-1), and AgNO3 (0.5 mmol L-1). (d) Control tests: air atmosphere, Ar atmosphere and O2 atmosphere. (e) •O2- was registered by EPR capture tests under photoirradiation. (f) In situ FT-IR spectra of 10%Ag-PCN/CdS-D in photocatalytic reaction.

Fig. 6. Electrostatic potentials of Ag-PCN (001) (a) and CdS-D (002) (b) surface. (c) Bader charge analysis of Ag-PCN absorbed with CdS-D. (d) The charge enrichment in yellow regions and charge consumption in cyan regions. (e) The charge migration pathway of S-scheme heterojunction.

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二维银修饰氮化碳/一维二乙烯三胺改性硫化镉S-型异质结及其高效光催化产过氧化氢性能

2D Ag modified g-C₃N₄/1D CdS-diethylenetriamine S-scheme heterojunction with enhanced photocatalytic H₂O₂ production

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二维银修饰氮化碳/一维二乙烯三胺改性硫化镉S-型异质结及其高效光催化产过氧化氢性能

2D Ag modified g-C3N4/1D CdS-diethylenetriamine S-scheme heterojunction with enhanced photocatalytic H2O2 production

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2D Ag modified g-C₃N₄/1D CdS-diethylenetriamine S-scheme heterojunction with enhanced photocatalytic H₂O₂ production