g-C3N4上非对称镍单原子-氮空位双位点高效光催化CO2还原

doi:10.1016/S1872-2067(26)65255-2

催化学报 ›› 2027, Vol. 92: 206-218.DOI: 10.1016/S1872-2067(26)65255-2

g-C₃N₄上非对称镍单原子-氮空位双位点高效光催化CO₂还原

吴丽君^a^,¹, 夏瑜^a^,¹, 班朝刚^b^,^*(), 王阳^c, 王晓星^a, 阮璐洁^a, 张子龙^a, 杜耀函^a, 马江平^b, 胡丽^a, 冉昊迪^b, 张敖^a, 陶晓萍^a^,^d^,^*(), 甘立勇^a^,^d, 周小元^a^,^d

^a 重庆大学物理学院, 量子材料与器件研究中心, 重庆 401331
^b 香港理工大学应用物理系, 香港 999077
^c 重庆邮电大学光电工程学院, 重庆 400065
^d 重庆大学前沿交叉学科研究院, 重庆 400044

收稿日期:2026-02-15 接受日期:2026-04-14 出版日期:2027-01-02 发布日期:2026-10-30
通讯作者: *电子信箱: chaogang.ban@polyu.edu.hk (班朝刚),
xptao@cqu.edu.cn (陶晓萍).
作者简介:第一联系人：
¹共同第一作者.
基金资助:
国家自然科学基金杰青项目(52125103);中央高校基本科研业务费(2025CDJ-IAISYB-039);重庆市自然科学基金(CSTB2024NSCQ-MSX0991);重庆市自然科学基金(CSTB2023NSCQ-MSX0394);国家外国专家项目(Y20240231);国家自然科学基金(22302023)

Asymmetric nickel single-atom and nitrogen vacancy dual sites on g-C₃N₄ for efficient CO₂ photoreduction to CO

Lijun Wu^a^,¹, Yu Xia^a^,¹, Chaogang Ban^b^,^*(), Yang Wang^c, Xiaoxing Wang^a, Lujie Ruan^a, Zilong Zhang^a, Yaohan Du^a, Jiangping Ma^b, Li Hu^a, Haodi Ran^b, Ao Zhang^a, Xiaoping Tao^a^,^d^,^*(), Liyong Gan^a^,^d, Xiaoyuan Zhou^a^,^d

^a College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, China
^b Department of Applied Physics, The Hong Kong Polytechnic University, Hong Kong 999077, China
^c School of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China
^d Institute of Advanced Interdisciplinary Studies, Chongqing University, Chongqing 400044, China

Received:2026-02-15 Accepted:2026-04-14 Online:2027-01-02 Published:2026-10-30
Contact: *E-mail: chaogang.ban@polyu.edu.hk (C. G. Ban),
xptao@cqu.edu.cn (X. P. Tao).
About author:First author contact:
¹ Contributed equally to this work.
Supported by:
National Natural Science Foundation of China for Distinguished Young Scholars of China(52125103);Fundamental Research Funds for the Central Universities(2025CDJ-IAISYB-039);Natural Science Foundation of Chongqing(CSTB2024NSCQ-MSX0991);Natural Science Foundation of Chongqing(CSTB2023NSCQ-MSX0394);National Young Foreign Talents Plan(Y20240231);National Natural Science Foundation of China(22302023)

摘要/Abstract

摘要：

光催化CO₂还原反应利用太阳能驱动CO₂转化为高附加值碳基化学品, 是实现人工碳循环与太阳能转化的重要途径. 其中, 以纯水作为唯一电子供体和质子源的无牺牲剂光催化全水解体系, 具备环境友好、成本低廉等优势, 被认为是最具可持续发展潜力的CO₂转化模式之一. 然而, 该体系的实际应用仍面临严峻的物理化学挑战: 一方面, 光生载流子极易快速复合, 导致其实际参与反应的效率较低; 另一方面, 该过程必须在严苛的热力学限制下, 利用光生载流子同时驱动动力学极其迟缓的水氧化反应(OER)以及高度稳定CO₂分子的活化. 两个半反应在时空尺度上难以实现有效的电荷匹配与动力学协同, 严重制约了整体反应的能量转化效率与目标产物选择性. 因此, 构筑兼具高效电荷分离能力与多底物协同活化功能的新型催化体系, 是提升纯水体系CO₂光还原性能的关键.

本文以石墨相氮化碳(g-C₃N₄)为模型光催化剂, 结合缺陷工程与单原子锚定策略, 成功构筑了由Ni单原子与氮空位协同驱动的非对称双位点催化体系(Ni₁-N_V/CN), 实现了纯水体系中CO₂的高效光还原. 该催化体系中, Ni单原子特异性地作为CO₂吸附与活化位点, 而相邻氮空位则作为H₂O吸附与解离位点, 二者在空间上形成分工明确的双活性位点界面, 实现了CO₂还原与H₂O氧化两个半反应的高效耦合. 性能评估表明, 在无牺牲剂的纯水和可见光照射条件下, Ni₁-N_V/CN表现出卓越的光催化CO₂还原性能, 其CO生成速率达到55.32 μmol g^-1 h^-1, 相较于单一氮缺陷的氮化碳(N_V/CN)提升8.3倍, 且保持了优异的CO产物选择性. 进一步机理研究揭示, Ni单原子与氮空位之间的电子强相互作用有效重塑了局域电子结构, 不仅显著促进了光生载流子的定向迁移与空间分离, 从源头上抑制了电子-空穴对的复合; 更重要的是, 这种空间协同效应优化了质子耦合电子转移(PCET)过程, 大幅降低了*COOH形成的自由能势垒, 从而加快CO生成反应动力学.

综上, 本研究构筑了一种面向纯水体系CO₂光还原的非对称双位点催化模型, 揭示了金属单原子与缺陷位点协同促进CO₂与H₂O活化的内在机制. 该工作不仅为纯水体系中多底物协同转化提供了新思路, 也为高效太阳能驱动CO₂资源化利用材料的理性设计提供了理论依据.

关键词: 非对称双位点, CO₂光还原, g-C₃N₄, Ni单原子, 氮空位

Abstract:

Photocatalytic CO₂ reduction using pure water offers a sustainable route for solar‐to‐fuel conversion, yet its efficiency is limited by sluggish charge separation and the insufficient activation of CO₂ and H₂O. Here, we construct asymmetric dual sites on graphitic carbon nitride by coupling nickel single atoms with nitrogen vacancies (Ni₁-N_V/CN). The optimized catalyst achieves an outstanding CO production rate of 55.32 μmol g^-1 h^-1 without sacrificial agents, representing an 8.3-fold enhancement over the nitrogen-deficient graphitic carbon nitride (N_V/CN) with excellent CO selectivity. Mechanistic investigations reveal a clear functional asymmetry: Ni single atoms serve as high-affinity centers for CO₂ adsorption and activation, whereas nitrogen vacancies promote H₂O adsorption and proton generation. This spatial cooperation accelerates proton-coupled electron-transfer steps, enhances charge separation, and substantially lowers the free-energy barrier for *COOH formation. This work establishes asymmetric dual-site engineering as an effective strategy for activating multi-molecule substrates in photocatalytic CO₂ conversion and offers mechanistic insights for designing advanced metal-defect architectures.

Key words: Asymmetric dual sites, CO2 photoreduction, g-C3N4, Ni single atoms, Nitrogen vacancy

吴丽君, 夏瑜, 班朝刚, 王阳, 王晓星, 阮璐洁, 张子龙, 杜耀函, 马江平, 胡丽, 冉昊迪, 张敖, 陶晓萍, 甘立勇, 周小元. g-C₃N₄上非对称镍单原子-氮空位双位点高效光催化CO₂还原[J]. 催化学报, 2027, 92: 206-218.

Lijun Wu, Yu Xia, Chaogang Ban, Yang Wang, Xiaoxing Wang, Lujie Ruan, Zilong Zhang, Yaohan Du, Jiangping Ma, Li Hu, Haodi Ran, Ao Zhang, Xiaoping Tao, Liyong Gan, Xiaoyuan Zhou. Asymmetric nickel single-atom and nitrogen vacancy dual sites on g-C₃N₄ for efficient CO₂ photoreduction to CO[J]. Chinese Journal of Catalysis, 2027, 92: 206-218.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65255-2

https://www.cjcatal.com/CN/Y2027/V92/I1/206

图/表 6

Fig. 1. XRD patterns (a) and FTIR spectra (b) of NV/CN and Ni1-NV/CN. (c) TEM image of Ni1-NV/CN. AC HAADF-STEM (d) and elemental mapping (e) images of Ni1-NV/CN.

Fig. 2. (a) EPR spectra of CN, NV/CN and Ni1-NV/CN. C 1s (b) and N 1s (c) XPS spectra of NV/CN and Ni1-NV/CN. Ni K-edge XANES (d) and FT-EXAFS R space (e) spectra for Ni1-NV/CN, Ni foil and NiPc. (f) FT-EXAFS R space fitting curves for Ni1-NV/CN. Wavelet transform plots for Ni foil (g), NiPc (h), and Ni1-NV/CN (i).

Fig. 3. (a) Time-dependent CO production over different photocatalysts. (b) Performance of photocatalytic CO2 reduction on Ni1-NV/CN as a function of Ni loading mass. (c) Product selectivity of CH4 and CO on CN, NV/CN and Ni1-NV/CN, respectively. (d) Cycling stability test of the Ni1-NV/CN.

Fig. 4. (a) UV-vis DRS and the corresponding Tauc plots (inset) of NV/CN and Ni1-NV/CN. Mott-Schottky plots of NV/CN (b) and Ni1-NV/CN (c). (d) Schematic diagram of the energy band structure. Carrier concentration (e), PL (f), TRPL (g), photocurrent response (h), and EIS plots (i) of NV/CN and Ni1-NV/CN.

Fig. 5. (a, b) In-situ DRIFTS of CO2 photoreduction over NV/CN and Ni1-NV/CN. (c) Density of states of CN, NV/CN and Ni1-NV/CN. (d) Differential charge density of Ni1-NV/CN. (e, f) Adsorption configurations of CO2 on the Ni site and H2O on the NV site in Ni1-NV/CN, respectively. (g) Adsorption energies of CO2 and H2O at the Ni single atom site and NV site on Ni1-NV/CN, respectively. (h) Gibbs free energy diagrams of CO2 photoreduction to CO for CN, NV/CN, and Ni1-NV/CN.

Fig. 6. The reaction mechanism for photocatalytic CO2 reduction on Ni1-NV/CN.

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g-C₃N₄上非对称镍单原子-氮空位双位点高效光催化CO₂还原

Asymmetric nickel single-atom and nitrogen vacancy dual sites on g-C₃N₄ for efficient CO₂ photoreduction to CO

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