单/双金属中心锚定在氮化碳: 温室气体转化和有机光合成的可持续路线

doi:10.1016/S1872-2067(26)65008-5

催化学报 ›› 2026, Vol. 85: 13-33.DOI: 10.1016/S1872-2067(26)65008-5

单/双金属中心锚定在氮化碳: 温室气体转化和有机光合成的可持续路线

兰青^a, 靳素娟^a, 焦莹莹^b^,^c(), 张志明^b()

^a 南阳师范学院化学与制药工程学院, 河南省太阳能催化工程技术研究中心, 河南南阳 473061
^b 天津理工大学材料科学与工程学院, 新能源材料与低碳技术研究所, 天津 300384
^c 郑州师范学院化学化工学院, 河南郑州 450044

收稿日期:2025-08-21 接受日期:2025-12-09 出版日期:2026-06-18 发布日期:2026-05-18
通讯作者: *电子信箱: yyjiao0210@163.com (焦莹莹),
zmzhang@email.tjut.edu.cn (张志明).
基金资助:
国家自然科学基金(92580109);天津市自然科学基金(25JCZDJC00570);河南省自然科学基金(252300423754);河南省自然科学基金(262102321040);河南省高校重点科研项目(26A150049);河南省高校重点科研项目(26B430036);河南省高校重点科研项目(24B430015);南阳市科技计划科技研发项目(24KJGG106);南阳师范学院专项项目(2024PY003)

Anchoring single/dual metal centers on carbon nitride: Sustainable routes for greenhouse gas conversion and organic photosynthesis

Qing Lan^a, Su-Juan Jin^a, Ying-Ying Jiao^b^,^c(), Zhi-Ming Zhang^b()

^a Engineering Technology Research Center of Henan Province for Solar Catalysis, College of Chemistry and Pharmaceutical Engineering, Nanyang Normal University, Nanyang 473061, Henan, China
^b Institute of New Energy Materials & Low Carbon Technology, School of Materials Science & Engineering, Tianjin University of Technology, Tianjin 300384, China
^c College of Chemistry and Chemical Engineering, Zhengzhou Normal University, Zhengzhou 450044, Henan, China

Received:2025-08-21 Accepted:2025-12-09 Online:2026-06-18 Published:2026-05-18
Contact: *E-mail: yyjiao0210@163.com (Y. Jiao),
zmzhang@email.tjut.edu.cn (Z. Zhang).
About author:Ying-Ying Jiao (Tianjin University of Technology, Institute for New Energy Materials and Low Carbon Technologies) obtained her PhD degree from Zheng-zhou University. From 2022 to 2023, she studied at the Polytechnic University of Valencia in Spain as an exchange student. In 2023, she joined the Institute for New Energy Materials and Low Carbon Technologies, Tianjin University of Technology. Her research interests focus on the application of carbon nitride based semiconductor materials in the field of photocatalysis.
Zhi-Ming Zhang (Tianjin University of Technology, Institute for New Energy Materials and Low Carbon Technologies) received the PhD degree in inorganic chemistry from Northeast Normal University in 2010. He was an iCHEM fellow at Xiamen University, and a visiting scholar at University of Chicago during 2013–2015. His research focuses on controlled synthesis of clusters, catalyst@photosensitiser composite catalytic systems. He has published over 150 peer-reviewed papers, such as Nat. Synth., PANS, Natl. Sci. Rev., CCS Chem, J. Am. Chem. Soc., Angew. Chem., Nat. Commun. and Adv. Mater. with over 10000 times citations, in which 12 papers are listed as highly cited papers by ESI.
Supported by:
National Natural Science Foundation of China(92580109);Natural Science Foundation of Tianjin City of China(25JCZDJC00570);Natural Science Foundation of Henan Province(252300423754);Natural Science Foundation of Henan Province(262102321040);Key Science Research Project of Colleges and Universities in Henan Province(26A150049);Key Science Research Project of Colleges and Universities in Henan Province(26B430036);Key Science Research Project of Colleges and Universities in Henan Province(24B430015);Science and Technology Research Project of Nanyang City's Science and Technology Plan(24KJGG106);Special Project of Nanyang Normal University(2024PY003)

摘要/Abstract

摘要：

全球经济与工业的快速发展造成了严重的温室效应, 导致了严峻的环境问题. 光催化二氧化碳还原和甲烷氧化制备增值化学品是兼具环境治理与能源供给效应的前沿技术, 它以清洁、可再生的光能为驱动力, 不仅能有效转化利用大气中的温室气体, 降低其浓度以缓解温室效应, 还能将这些原本的“环境负担”转化为甲醇、甲酸、烯烃等高价值燃料或化工原料, 既为解决能源短缺问题开辟了新路径, 又实现了“碳减排”与“资源增值”的双重目标, 对推动可持续发展具有深远意义.

本文系统综述了石墨相氮化碳(g-C₃N₄)基单原子催化剂(SACs)与双原子催化剂(DACs)在温室气体转化和有机光合成领域的最新研究进展. 基于g-C₃N₄独特的共轭结构、可调的电子特性以及优异的光化学稳定性, 重点围绕催化剂的设计思路与合成方法展开深入探讨, 既涵盖了高温热解、湿化学沉积和光还原等传统制备策略的优化升级, 也囊括了模板辅助合成等新型技术的创新应用. 在反应机理层面, 结合先进的原位表征技术与理论计算模拟, 详细剖析了g-C₃N₄载体与单/双金属活性位点之间的电子传递路径、中间体吸附-脱附行为, 以及催化反应的决速步骤. 同时, 聚焦催化剂的实际应用场景, 全面阐述了其在温室气体转化和有机光合成中的性能表现与构效关系. 此外, 本文进一步强调了该研究领域的三大前沿发展趋势: (1)借助球差校正电子显微镜、同步辐射等高级表征手段, 实现对原子级活性位点的精准识别与动态监测; (2)发展精密合成技术, 精准调控活性金属原子的配位环境与空间分布, 提升催化剂的选择性与稳定性; (3)深入阐明金属-载体相互作用机制, 为高效催化剂的理性设计提供理论支撑, 最终为该领域的后续研究指明了清晰且具有前瞻性的方向.

综上, g-C₃N₄基SACs/DACs制备存在金属负载量较低、分散难等问题, 需要开发新的合成策略; DACs具有协同优势, 却面临结构调控、合成表征等挑战; 温室气体转化研究尚处起步阶段, 目前产物多为C₁化合物, 多碳及含氮化合物合成仍是关键难题. 期待本文激发相关研究人员深入思考, 并进一步推动光催化技术在温室气体转化和有机光合成领域中的实际应用.

关键词: 单/双原子, 金属中心, 氮化碳, 温室气体转化, 有机光合成

Abstract:

Single-atom and dual-atom catalysts (SACs/DACs) have attracted significant interest owing to their maximized atom utilization efficiency and distinctive synergistic properties. Nevertheless, the fabrication of highly efficient and stable SACs/DACs continues to present considerable challenges, largely due to elevated surface energy and the complexity of achieving precise coordination environments and spatial distribution of metallic sites. Effective regulation of chemical bonding between metal centers and supporting matrices is crucial to suppress aggregation tendencies. Carbon nitride (g-C₃N₄) has gained prominence as a robust scaffold for immobilizing SACs and DACs, attributed to its well-defined electronic configuration, notable chemical stability, and customizable surface characteristics. A dynamic electronic interplay is observed: metal species tailor the electronic properties of g-C₃N₄, while the support reciprocally modulates the catalytic behavior of metal active sites. This review comprehensively outlines recent progress in g-C₃N₄-based SACs and DACs, with focused discussion on synthetic methodologies, reaction mechanisms, and applications in greenhouse gas transformation and photosynthetic organic synthesis. Furthermore, the article emphasizes emerging trends in advanced characterization, precision synthesis, and the elucidation of bidirectional metal-support interactions, offering insightful directions for subsequent research in the field.

Key words: Single/dual atom, Metal centers, Carbon nitride, Greenhouse gas conversion, Organic photosynthesis

兰青, 靳素娟, 焦莹莹, 张志明. 单/双金属中心锚定在氮化碳: 温室气体转化和有机光合成的可持续路线[J]. 催化学报, 2026, 85: 13-33.

Qing Lan, Su-Juan Jin, Ying-Ying Jiao, Zhi-Ming Zhang. Anchoring single/dual metal centers on carbon nitride: Sustainable routes for greenhouse gas conversion and organic photosynthesis[J]. Chinese Journal of Catalysis, 2026, 85: 13-33.

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图/表 19

Fig. 1. The development and statistics of g-C?N?-supported SACs and DACs. (a) The number of publications between 2020 and 2025. (b) The number of citations each year.

Fig. 2. g-C3N4-supported SACs and DACs schematic diagram according to the summary of time development.

Fig. 3. Synthesis strategies for g-C3N4-based SACs/DACs.

Fig. 4. (a) Schematic illustration of the preparation of Fe-g-C3N4 SACs. STEM (b), AC-HAADF-STEM (c), and corresponding EDX elemental mapping (d) images of Fe-g-C3N4 SACs. Reprinted with permission from Ref. [43]. Copyright 2022, Elsevier.

Fig. 5. Characterization of SACo/g-C3N4. (a) SEM image of SACo/g-C3N4, and the inset shows the optical image of 1.1 g SACo/g-C3N4. TEM (b) and HAADF-STEM (c) images of SACo/g-C3N4. (d) HAADF and the corresponding EDS mapping images of SACo/g-C3N4, the scale bar is 100 nm. HRTEM (e) and AC-STEM-annular dark field (ADF) (f) images of SACo/g-C3N4. Reprinted with permission from Ref. [55]. Copyright 2021, RSC.

Fig. 6. Physical characterization of Ni-g-C3N4. (a) Schematic illustration of the preparation. SEM (b), HRTEM (c), AC HAADF-STEM (d), and EDS mapping (e) images. Reprinted with permission from Ref. [62]. Copyright 2022, Nature.

Fig. 7. (a) Schematic illustration of the synthesis process of Cu SACs/g-C3N4 photocatalyst. TEM (b), HRTEM (c), and AC STEM (d) images of Cu SACs/g-C3N4. Cu single atoms were marked with red circles. (e) Elemental mapping image of Cu SACs/g-C3N4. Reprinted with permission from Ref. [59]. Copyright 2021, Wiley.

Fig. 8. (a) Schematic diagram of catalyst synthesis processes. (b) Typical time course of CO evolution catalyzed by g-C3N4-CoxNiy and the photocatalytic CO2 reduction mechanism in this system. Reprinted with permission from Ref. [73]. Copyright 2022, Elsvier.

Fig. 9. Two-step strategy for the precise synthesis of heteronuclear DACs. (a) A schematic illustration of the navigation and positioning strategy for fabricating ZnRu-, NiRu-, ZnCu-, CoCu-, NiCu- and BiCu-g-C3N4 heteronuclear DACs. (b) Photocatalytic H2 evolution in H2O in the presence of LA. (c) PA production of ZnRu-g-C3N4 and control samples. (d) A schematic diagram of photocatalysis process (grey, blue, pink and green balls represent C, N, Ru and Zn, respectively). Reprinted with permission from Ref. [75]. Copyright 2024, Nature.

Table 1 Summary of various applications of g-C3N4-based SACs/DACs.

Photo catalyst	Fabricating method	Application	Photocatalyst eﬃciency	Production	Characteristic	Advantages	Ref.
Co-SNC	ball-milling	benzylamine self-coupling reaction	97.5% conversion with 99% selectivity	N-benzylidene-benzylamine	high-performance dual-site SACs	high selectivity	[18]
W-SA-PCN	calcining	CH₄ Photooxidation	4956 µmol·g_cat^∙1	C₁ oxygenates	WN₄ coordination mode	high productivity	[79]
Cu-CCN	molten salts	CO₂ photoreduction	3.086 μmol·h^∙1·g^∙1	CO	crystalline g-C₃N₄ accompanied with Cu ions	highly selectivity	[36]
Cu/CN	supramolecular preorganization with subsequent condensation,	CO₂ photoreduction	224.2 μmol∙h^∙1∙g^∙1	CO	C-Cu-N₂ SAC for CO₂ activation	high CO-selectivity	[84]
PCN-RuCu	preassembly-coprecipitation-pyrolysis	CO₂ Photoreduction	19.25 µmol· g^-1·h^-1	CH₄	Ru sites account for electron-hole pairs and Cu sites for CO₂ hydrogenation	high selectivity of 95%	[91]
Ag₁(x)@PCN	impregnation and pyrolysis	CO₂ photoreduction	160 μmol·h^∙1·g^∙1	CO	Ag single atoms anchored on hollow porous polygonal C₃N₄ tubes	excellent stability	[51]
M₁M₂-PCN DACs	photoinduced strategy	Photocatalytic H₂ evolution	345 mmol∙ g_Ru^∙1∙h^∙1	H₂	anchoring heteronuclear dual-metal dimers on a photosensitizing PCN to construct a series of DACs	bimetallic precise identification	[75]
RuSA-mC₃N₄	SBA-15	CO₂ photoreduction	250 μmol·h^∙1·g^∙1	Methanol	Ruthenium single atom over mesoporous C₃N₄	high methanol yield	[82]
CoRu-HCNp	self-seeded process with condensation and carbonization	CO₂ photoreduction	27.3 µmol·g^-1·h^-1	CO	Conjugated porous carbon nitride polymer with precise control of Co-Ru atomic configuration	High CO-selectivity	[94]
Pd₁+NPs/ C₃N₄	calcining	CO₂ photoreduction	20.3 µmol·g^-1·h^-1	CH₄	Pd₁ sites activated CO₂ and PdNPs sites increased H* coverage	high selectivity of 97.8%	[92]

Table 1 Summary of various applications of g-C3N4-based SACs/DACs.

Photo catalyst	Fabricating method	Application	Photocatalyst eﬃciency	Production	Characteristic	Advantages	Ref.
Co-SNC	ball-milling	benzylamine self-coupling reaction	97.5% conversion with 99% selectivity	N-benzylidene-benzylamine	high-performance dual-site SACs	high selectivity	[18]
W-SA-PCN	calcining	CH₄ Photooxidation	4956 µmol·g_cat^∙1	C₁ oxygenates	WN₄ coordination mode	high productivity	[79]
Cu-CCN	molten salts	CO₂ photoreduction	3.086 μmol·h^∙1·g^∙1	CO	crystalline g-C₃N₄ accompanied with Cu ions	highly selectivity	[36]
Cu/CN	supramolecular preorganization with subsequent condensation,	CO₂ photoreduction	224.2 μmol∙h^∙1∙g^∙1	CO	C-Cu-N₂ SAC for CO₂ activation	high CO-selectivity	[84]
PCN-RuCu	preassembly-coprecipitation-pyrolysis	CO₂ Photoreduction	19.25 µmol· g^-1·h^-1	CH₄	Ru sites account for electron-hole pairs and Cu sites for CO₂ hydrogenation	high selectivity of 95%	[91]
Ag₁(x)@PCN	impregnation and pyrolysis	CO₂ photoreduction	160 μmol·h^∙1·g^∙1	CO	Ag single atoms anchored on hollow porous polygonal C₃N₄ tubes	excellent stability	[51]
M₁M₂-PCN DACs	photoinduced strategy	Photocatalytic H₂ evolution	345 mmol∙ g_Ru^∙1∙h^∙1	H₂	anchoring heteronuclear dual-metal dimers on a photosensitizing PCN to construct a series of DACs	bimetallic precise identification	[75]
RuSA-mC₃N₄	SBA-15	CO₂ photoreduction	250 μmol·h^∙1·g^∙1	Methanol	Ruthenium single atom over mesoporous C₃N₄	high methanol yield	[82]
CoRu-HCNp	self-seeded process with condensation and carbonization	CO₂ photoreduction	27.3 µmol·g^-1·h^-1	CO	Conjugated porous carbon nitride polymer with precise control of Co-Ru atomic configuration	High CO-selectivity	[94]
Pd₁+NPs/ C₃N₄	calcining	CO₂ photoreduction	20.3 µmol·g^-1·h^-1	CH₄	Pd₁ sites activated CO₂ and PdNPs sites increased H* coverage	high selectivity of 97.8%	[92]

Fig. 10. Calculated PDOS of g-C3N4 (a) and In1/g-C3N4 (b). (c) Calculated Gibbs free energy diagram for CO2 reduction pathways to CO on g-C3N4, In1/g-C3N4 and Co1/g-C3N4. (d) Computed Gibbs free energy for steps in photocatalytic *CO-to-CHO on g-C3N4, In1/g-C3N4 and Co1/g-C3N4. (e) Calculated Gibbs free energy diagram for CO2 reduction pathways to CH4 on Co1In1/g-C3N4. Reprinted with permission from Ref. [61]. Copyright 2025, Elsevier.

Fig. 11. (a) EXAFS spectra of Co K-edge for Co foil, Co3O4 and Co1In1/g-C3N4. (b) Co K-edge FT-EXAFS spectra. (c) EXAFS spectra of In K-edge for In foil, In2O3 and Co1In1/g-C3N4. (d) In K-edge FT-EXAFS spectra. In-situ DRIFTS spectra at different irradiation times on g-C3N4 (e) and Co1In1/g-C3N4 (f). Reprinted with permission from Ref. [61]. Copyright 2025, Elsevier.

Fig. 12. (a) HAADF-STEM image of W-SA-g-C3N4-7.5 showing the W-single-atom distribution on g-C3N4, (b) CH3OH yield of SAP and control samples, (c) Time-course plots of CH3OH yield, and (d) DFT calculations results for CH4 oxidation with W-SA-g-C3N4-7.5 as the photocatalyst. Reprinted with permission from Ref. [79]. Copyright 2022, Wiley.

Fig. 13. TEM images and synchrotron radiation analysis of g-C3N4 and Cu/g-C3N4 samples. TEM (a), (b) HADDF-STEM, and (c) EDS elemental mapping images of Cu/g-C3N4-3. (d) FT-EXAFS and (e) XANES spectra of Cu K-edge for the Cu/g-C3N4 samples with Cu foil, Cu2O and CuO as the references. (f) CO2 photoreduction performance of g-C3N4 and Cu/g-C3N4 at the first hour of irradiation. (g) Time courses of photocatalytic activities of Cu/g-C3N4-0.25 and (h) GC-MS analysis of reaction products with 12C and 13C as carbon source, respectively. Reprinted with permission from Ref. [84]. Copyright 2020, American Chemical Society.

Fig. 14. (a) Schematic illustration of synthetic procedure for PtCu-g-C3N4. (b) AC-HAADF-STEM images of PtCu-g-C3N4 (the right shows partially zoomed-in images of the selected region 2, and corresponding intensity pro?le along the labeled line 1; scale bar: 0.1 nm). (c) The Cu and Pt contents measured by ICP-MS test. (d) Comparable photocatalytic yield for CO of PtCu-g-C3N4, Cu-g-C3N4, Pt-g-C3N4, and g-C3N4 under simulated solar illumination. Reprinted with permission from Ref. [93]. Copyright 2022, Elsevier.

Fig. 15. (a) Schematic illustration of the developed ball-milling approach. (b) HAADF-STEM/EDX-mapping images of Co-SNC and Co-NC. (c-f) Catalytic performance of Co-SNC in benzylamine self-coupling reaction. Reprinted with permission from Ref. [18]. Copyright 2021, Wiley-VCH.

Fig. 16. (a) Diagrammatic illustration of the preparation of Ni-SA/g-C3N4. (b) Representative HAADF-STEM image. (c) The intensity pro?les obtained in regions 1 and 2 in (b). (d) TEM and matching EDS elemental mapping images of Ni-SA/g-C3N4, (e) Oxidative imine formation catalyzed by a Ni SAC. Reprinted with permission from Ref. [99]. Copyright 2022, American Chemical Society.

Fig. 17. Photocatalytic applications of g-C3N4-based SACs and DACs.

Fig. 18. Future perspectives of g-C3N4-based SACs and DACs.

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单/双金属中心锚定在氮化碳: 温室气体转化和有机光合成的可持续路线

Anchoring single/dual metal centers on carbon nitride: Sustainable routes for greenhouse gas conversion and organic photosynthesis

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