物理化学学报 >> 2026, Vol. 42 >> Issue (10): 100264.doi: 10.1016/j.actphy.2026.100264

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分级ZIF衍生碳/Bi12O17Cl2异质结构协同调控电子动力学与光学性能,提升纯水体系中CO2光还原性能

高韵晗1, 孙星2, 季梦夏1,*(), 邱杏昌1, 韦天歌1, 徐箐2, 尹盛2, 夏杰祥2,*(), 李华明1,*()   

  1. 1 江苏大学能源研究院, 江苏 镇江 212013
    2 江苏大学化学化工学院, 江苏 镇江 212013
  • 收稿日期:2025-12-03 修回日期:2026-02-16 录用日期:2026-02-25 发布日期:2026-09-03
  • 通讯作者: Email: jmx@ujs.edu.cn (季梦夏)xjx@ujs.edu.cn (夏杰祥)lihm@ujs.edu.cn (李华明)

Hierarchical ZIF-derived carbon/Bi12O17Cl2 heterostructures synergistically enhance electron dynamics and optical properties to boost CO2 photoreduction in pure water

Yunhan Gao1, Xing Sun2, Mengxia Ji1,*(), Xingchang Qiu1, Tiange Wei1, Qing Xu2, Sheng Yin2, Jiexiang Xia2,*(), Huaming Li1,*()   

  1. 1 Institute for Energy Research, Jiangsu University, Zhenjiang 212013, Jiangsu Province, China
    2 School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu Province, China
  • Received:2025-12-03 Revised:2026-02-16 Accepted:2026-02-25 Published:2026-09-03
  • Contact: Email: jmx@ujs.edu.cn (Mengxia Ji)xjx@ujs.edu.cn (Jiexiang Xia)lihm@ujs.edu.cn (Huaming Li)

摘要:

传统Bi12O17Cl2光催化剂存在太阳光捕获范围窄、CO2吸附能力弱及电荷利用率低等问题。本研究通过将Bi12O17Cl2超薄纳米管嵌入分级Co-ZIF衍生多孔碳(Co-PC/BOC),构建了紧密的分级异质结结构。Co-PC纳米笼内的多重空腔反射效应与原位生成Co3O4位点的局域表面等离子体共振协同作用,使Co-PC/BOC在全光谱范围内光捕获能力显著增强。在不使用任何光敏剂或牺牲剂的纯水体系中,最优复合材料表现出34.16 μmol g−1 h−1的CO产率(100%选择性),是单体BOC的2.9倍。原位漫反射红外光谱及光电化学测试表明:Co-PC兼具等离子体热电子注入体与电荷分离中心的双重功能,而BOC为*COOH形成与*CO解离提供了丰富的表面活性位点。本工作揭示了金属有机框架及其衍生物在构建高效人工光合体系中的重要潜力。

关键词: Bi12O17Cl2纳米管, MOFs衍生物, 电荷分离, 等离子体共振, CO2光还原

Abstract:

Conventional Bi12O17Cl2 photocatalyst suffer from narrow solar harvesting, weak CO2 adsorption and poor charge utilization. Herein, an intimate hierarchical heterojunction was constructed by embedding Bi12O17Cl2 ultrathin nanotubes into hierarchical Co-ZIF-derived porous carbon (Co-PC/BOC). Multi-cavity reflection within Co-PC nanocages and localized surface plasmon resonance of in situ generated Co3O4 domains synergistically enhance the light harvest ability of the Co-PC/BOC in the full spectral range. In pure water without any photosensitizers or sacrificial agents, the optimal composite exhibits a CO yield of 34.16 μmol g−1 h−1 with 100% selectivity, 2.9-fold higher than bare BOC. In situ DRIFTS and photo/electrochemical characterizations demonstrate that Co-PC serves as a dual-function platform of plasmonic hot-electron injector and charge separation hub, whereas BOC provide abundant surface sites for *COOH formation and *CO cleavage. Our work highlights the promising potential of metal-organic frameworks and their derivatives in developing efficient artificial photosynthesis systems.

Key words: Bi12O17Cl2 nanotube, MOFs derivative, Charge separation, Plasmon resonance, CO2 photoreduction