二维(2D)材料上的单原子催化剂用于光催化CO2还原: 基础、设计与新兴策略

doi:10.1016/S1872-2067(26)65135-2

催化学报 ›› 2026, Vol. 88: 86-128.DOI: 10.1016/S1872-2067(26)65135-2

二维(2D)材料上的单原子催化剂用于光催化CO₂还原: 基础、设计与新兴策略

Sathi Chatterjee^a, 李红梅^a, 刘康^a, 林璋^b, 柴立元^b, 刘敏^a^,^b^,^*()

^a 中南大学物理学院, 湖南二氧化碳资源化利用联合国际研究中心, 湖南长沙 410083
^b 中南大学冶金与环境学院, 湖南长沙 410083

收稿日期:2025-12-22 接受日期:2026-02-28 出版日期:2026-09-18 发布日期:2026-09-05
通讯作者: *电子信箱: minliu@csu.edu.cn (刘敏).
基金资助:
国家重点研发计划(2024YFC3712104);国家科技重大专项(2025ZD1204304);国家自然科学基金创新研究群体项目(52121004);国家自然科学基金(G22376222);国家自然科学基金(22403108);湖南省科技重大专项(2023RC1012);湖南省自然科学基金(2024JJ6484);中南大学前沿交叉学科研究计划(2023QYJC012)

Single-atom catalysts on two-dimensional (2D) materials for photocatalytic CO₂ reduction: Fundamentals, design, and emerging strategies

Sathi Chatterjee^a, Hongmei Li^a, Kang Liu^a, Zhang Lin^b, Liyuan Chai^b, Min Liu^a^,^b^,^*()

^a Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, School of Physics, Central South University, Changsha 410083, Hunan, China
^b School of Metallurgy and Environment, Central South University, Changsha 410083, Hunan, China

Received:2025-12-22 Accepted:2026-02-28 Online:2026-09-18 Published:2026-09-05
About author:Min Liu (Central South University) received his PhD (2010) degree from the Institute of Electrical Engineering, Chinese Academy of Sciences. In 2010-2015, he worked in University of Tokyo as a postdoctoral fellow with the guidance of Prof. Kazuhito Hashimoto and Prof. Kazunari Domen. In 2015-2017, he joined the University of Toronto as a postdoctoral fellow under the guidance of Prof. Edward Sargent. Since 2017, he is a professor in Central South University. His research interests focus on greenhouse gas reduction and energy catalysis, including the resource utilization of perfluorocarbon, electrocatalytic CO₂ reduction, and photo(electro)chemical water splitting. He got a number of over 300 publications on Nature, Nat Catal, Nat Commun, Joule, J. Am. Chem. Soc., Angew. Chem. Int. Ed., Adv. Mater. Nano Lett., et al, with citations of over 40000 and H-factor of 101. The research results have been highlighted by Science Daily, Science news, Phys.org, Forbes and other media. Based on these researches, he was awarded as a highly cited researcher by Clarivate Analytics from 2020 to 2024.
Supported by:
The National Key R&D Program of China(2024YFC3712104);The National Science and Technology Major Project of China(2025ZD1204304);The Foundation for Innovative Research Groups of the National Natural Science Foundation of China(52121004);The National Natural Science Foundation of China(G22376222);The National Natural Science Foundation of China(22403108);The Science and Technology Innovation Program of Hunan Province(2023RC1012);The Natural Science Foundation of Hunan Province(2024JJ6484);The Central South University Research Programme of Advanced Interdisciplinary Studies(2023QYJC012)

摘要/Abstract

摘要：

随着大气中CO₂浓度的持续升高以及太阳燃料转化需求的不断增强, 利用太阳能驱动CO₂高效转化为燃料和高附加值化学品已成为能源与环境领域的重要研究方向. 然而, CO₂分子具有高度稳定的线性结构和较大的活化能垒, 其多电子/质子耦合还原过程复杂, 并易受到析氢反应(HER)的竞争影响, 导致传统光催化体系在活性、选择性和稳定性方面面临显著挑战. 单原子催化剂(SACs)因具备原子级分散活性中心与可调控配位环境, 在提高金属利用效率和调控反应路径方面展现出独特优势. 将单原子锚定于二维(2D)材料表面, 可结合二维载体的平面限域效应、缺陷结构调控能力及高效电荷传输通道, 为构建高性能光催化CO₂还原体系提供新的理论基础与材料设计思路.
本文系统综述了二维材料负载单原子催化剂(SAC/2D)在光催化CO₂还原中的研究进展与设计框架. 首先, 从CO₂活化的热力学与动力学基础出发, 分析不同还原产物所需的电位条件与能带匹配关系, 阐述多电子/质子耦合转移机制、自由基中间体形成路径及析氢反应竞争行为, 明确反应能垒与中间体稳定化在决定反应路径和产物分布中的关键作用. 随后, 总结单原子位点在二维载体上的构筑策略, 包括湿化学法、热解法、原子层沉积及限域调控等方法, 并讨论不同制备路径对单原子配位环境、锚定稳定性及活性位点暴露程度的影响. 在结构表征方面, 综述原子尺度直接成像、配位与价态分析、振动光谱表征及时间分辨载流子动力学测试等先进技术, 结合密度泛函理论计算, 建立单原子局域结构、电子结构调控与光催化性能之间的关联机制. 通过对碳基二维材料、金属氧化物二维材料及新兴二维载体体系的性能趋势进行比较分析, 揭示平面限域效应、载体极性调控、界面耦合强度及电荷传输行为在协同调控催化活性、C₁与C₂⁺产物选择性以及长期稳定性方面的重要作用. 在此基础上, 构建统一的SAC/2D光催化设计框架, 将原子配位环境、二维载体效应与界面电荷流调控整合为系统性设计原则, 并提出三类关键工程策略: 异核双原子位点构筑、异质结构界面设计以及内建电场与极化调控机制, 用以缓解单原子稳定性不足、多碳产物选择性偏低及载流子快速复合等问题, 同时为实现可重复高负载合成与器件化构型应用提供理论指导.
总体而言, 本综述构建了贯通基础机理、二维材料效应、性能规律与工程策略的系统框架, 明确SAC/2D体系在光催化CO₂还原中的优势与挑战. 未来研究需加强原位机理解析、提高C₂⁺产物选择性与长期稳定性, 并推动薄膜化与流动反应器等器件化发展, 以促进高效、稳定且可规模化的光催化CO₂资源化利用体系的实现.

关键词: 光催化二氧化碳还原, 单原子催化剂, 二维材料, 太阳燃料生成, C₂₊选择性

Abstract:

The rapid increase of the concentration of atmospheric CO₂ and the imperative for solar-fuel generation highlight the urgent need for advanced catalytic materials. Single-atom catalysts (SACs) anchored on two-dimensional (2D) materials present a powerful approach by combining atomically isolated active sites with tunable coordination environments, defect chemistry, and enhanced charge-transport pathways intrinsic to 2D supports. This review explores SAC/2D systems for photocatalytic CO₂ reduction, beginning with the fundamental thermodynamics and kinetics of CO₂ activation, multielectron proton-coupled transfer, hydrogen-evolution competition and C₁ vs. C₂⁺ product selectivity. Then, it covers synthesis strategies for anchoring atomically dispersed metal sites on 2D supports, and discusses advanced characterization techniques‒including atomic-scale imaging, operando coordination spectroscopy and time-resolved carrier-dynamics measurements; that link structure and photocatalytic function. Photocatalytic performance trends across carbon-based, metal-oxide and emerging 2D supports are analysed to illustrate how planar confinement, support polarity, interfacial coupling, and charge-carrier behaviour regulate activity, selectivity, and stability. Further, a unified design framework is established, and three framework-guided design strategies i.e., heteronuclear dual-atom sites, heterostructure interfaces and internal-field/polarization engineering, are highlighted as promising strategy to overcome several intrinsic and scale-up challenges i.e., single atom instability, low multicarbon (C₂⁺) selectivity and rapid recombination. Finally, by aligning mechanistic insight with material design and pointing toward reproducible high-loading synthesis and device-oriented configurations (e.g., thin-films, flow-reactors), the review outlines a pathway toward selective, stable and scalable SAC/2D photocatalyst systems for solar-driven CO₂ reduction.

Key words: Photocatalytic CO₂ reduction, single-atom catalysts, 2D materials, Solar fuel generation, C₂₊ selectivity

Sathi Chatterjee, 李红梅, 刘康, 林璋, 柴立元, 刘敏. 二维(2D)材料上的单原子催化剂用于光催化CO₂还原: 基础、设计与新兴策略[J]. 催化学报, 2026, 88: 86-128.

Sathi Chatterjee, Hongmei Li, Kang Liu, Zhang Lin, Liyuan Chai, Min Liu. Single-atom catalysts on two-dimensional (2D) materials for photocatalytic CO₂ reduction: Fundamentals, design, and emerging strategies[J]. Chinese Journal of Catalysis, 2026, 88: 86-128.

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图/表 26

Fig. 1. Outline diagram of the review.

Fig. 2. Photocatalytic CO2 reduction mechanism on SAC/2D photocatalysts.

Fig. 3. Representative reaction pathways for photocatalytic CO2 reduction showing key intermediates and routes leading to C1 and C2 products. Reproduced from Ref. [14]. Copyright 2022, The Authors. Published by American Chemical Society under the Creative Commons CC BY 4.0 license.

Fig. 4. Band edge (CBM and VBM) alignments related to vacuum for various M@2DPI systems (M = La, Ti, Y, Mn, V, Sc, Hf, Zr) from HSE06+SOC calculations. Reproduced from Ref. [88]. Copyright 2023, The Authors. Published by Elsevier B.V. Licensed under CC BY.

Fig. 5. Wet Chemical synthesis of high-loading MSAPs-PuCN (M = Fe, Co, Ni, Cu, Zn, Sr, W, Pt). Reproduced from Ref. [102]. Copyright 2023, The Authors. Published by Springer Nature. Licensed under CC BY.

Fig. 7. Atomic layer deposition (ALD) synthesis of Co single atom catalysts on graphene (Co1/G). Reproduced from Ref. [111]. Copyright 2018, The Authors. Published by Springer Nature. Licensed under CC BY.

Fig. 8. Schematic diagram of (a) 2D CeO2 supported atomic Pt catalysts prepared using the precursor combustion strategy. Reproduced from Ref. [105] with permission. Copyright 2024, John Wiley and Sons and (b) Ni loading on g-C3N4 synthesized via high-energy ball milling method. Reproduced from Ref. [115] with permission. Copyright 2022, Elsevier.

Fig. 9. (a) HAADF-STEM image of Fe single atoms on Ti3−xC2Ty (Fe atoms marked with red circles). (b) Magnified atomic-resolution HAADF-STEM image. (c) Intensity profiles of selected regions. Reproduced from Ref. [118] with permission. Copyright 2024, The Royal Society of Chemistry. (d,e) Filtered atomic-resolution HAADF-STEM color maps of Aun/Au1-CMS. Reproduced from Ref. [50] with permission. Copyright 2024, Springer Nature. (f) AC-HAADF-STEM image of Pt1@CN. Reproduced from Ref. [72] with permission. Copyright 2024, Elsevier.

Fig. 10. (a) HRTEM image and SAED pattern for Aun/Au1-CMS. Reproduced from Ref. [50] with permission. Copyright 2024, Springer Nature. (b) HRTEM image of Pd/Co3O4. Reproduced from Ref. [120] with permission. Copyright 2024, John Wiley and Sons. (c,d) HRTEM image of Cu-PCN. Reproduced from Ref. [121] with permission. Copyright 2024, American Chemical Society.

Fig. 11. (a) Diffusion of single Ni atom on graphene edge region. (b,f) High-speed STM images. (c,g) Laplace filtered images. (d,h) Constant-height STM simulation based on geometries (e,i). Reproduced from Ref. [123] with permission. Copyright 2018, The American Association for the Advancement of Science.

Fig. 12. (a) EDX map of Pt-SA-decorated TiO2 layer. Reproduced from Ref. [124]. Copyright 2020, The Authors. Published by Wiley Advanced. under the Creative Commons CC BY. (b) Element mapping results of Co-Ti3C2Tx (MXene) nanosheets. Reproduced from Ref. [37] with permission. Copyright 2021, Elsevier. (c,d) EDX elemental mapping profiles with W (green), Cu (orange), Pt (yellow), and O (blue) distribution of the Cu2Pt2/WO3 catalyst. Reproduced from Ref. [125] with permission. Copyright 2022, Elsevier.

Fig. 13. (a) Synchrotron radiation Cu K-edge XANES. (b) XAFS Bi L1-edge. (c) EXAFS spectra of Bi L1-edge. Reproduced from Ref. [128] with permission. Copyright 2022, John Wiley and Sons. (d) XANES and (e) FT-EXAFS curves at Ni K-edge. Reproduced from Ref. [129] with permission. Copyright 2021, Elsevier. (f) Co K-edge XANES spectra, (g) Fourier transform magnitudes of the experimental Co K-edge EXAFS spectra of BP-Co and reference samples. Reproduced from Ref. [130] with permission. Copyright 2020, John Wiley and Sons.

Fig. 14. High-resolution XPS spectra for the Cu/TiO2-2/24 h and Cu/TiO2-2 of Cu 2p region (a) and O 1s (b) region. Reproduced from Ref. [132]. Copyright 2019, The Authors. Published by John Wiley and Sons under the Creative Commons CC BY 4.0 license. High-resolution N 1s XPS spectra of COF-Py and COF-Py-Co (c), COF-Pz and COF-Pz-Co (d). (e) High-resolution Co 2p XPS spectra of COF-Py-Co and COF-Pz-Co. Reproduce from Ref. [133] with permission. Copyright 2025, Elsevier, (f) High-resolution XPS spectrum of N 1s in the ICN-16. Reproduced from Ref. [134] with permission. Copyright 2023, John Wiley and Sons. (g) Elemental content of Co-N-Gr obtained from XPS and ICP-AES measurements, and high-resolution N 1s XPS spectrum (inset) divided into five Voigt-type line-shaped peaks. (h) Schematic model of Co-N-Gr, including C (black), N (green), and Co (yellow) atoms. Reproduced from Ref. [135]. Copyright 2020, The Authors. Published by American Chemical Society under the Creative Commons CC BY 4.0 license.

Fig. 15. (a-c) HAADF images of a 2D Co3O4-supported La single-atom catalyst, where Co3O4 nanocrystallites are indicated by yellow arrows and isolated La atoms by red arrows; the corresponding EELS spectrum was acquired from a single supported La atom. Reproduced from Ref. [137] with permission. Copyright 2020, Oxford University Press, Comparison of conventional and DED STEM-EELS mapping for FeReNC. HAADF image (d) and conventional EELS map (e) of the Fe-L2,3 edge showing no distinct localization above the noise level, whereas HAADF image (f) and DED EELS map (g) clearly resolves individual Fe atomic sites. (h,i) Atomic positions obtained from HAADF and DED EELS confirm the presence and absence of the Fe-L2,3 edge at Fe and non-Fe sites, respectively. Reproduced from Ref. [138] with permission. Copyright 2023, Elsevier.

Fig. 16. (a) FTIR spectra of GO, Mn-NGO 10 and Mn-NGO 30. Reproduced from Ref. [140] with permission. Copyright 2023, Elsevier. (b) g-C3N4 and Co/ g-C3N4-0.2. Reproduced from Ref. [141] with permission. Copyright 2021, Elsevier.

Fig. 17. (a) In-situ DRIFT spectra recorded during the photocatalytic CO2 reduction over the Cu2+/GDYO nanosheets. Reproduced from Ref. [144] with permission. Copyright 2021, John Wiley and Sons. (b) In-situ DRIFTS detection of PdSA+NCs/CeO2. Reproduced from Ref. [145] with permission. Copyright 2025, American Chemical Society.

Fig. 19. (a) Time-resolved fluorescence decay spectra of Ru single atoms on a mesoporous carbon nitride network (RuSA-mC3N4). Adapted from Ref. [147] with permission. (b) TRPL spectra of Cu-O/N single sites incorporated into a COF. Adapted from Ref. [150] with permission.

Fig. 21. Calculated Bader charge distribution at the Ru NP/GO interface (a) and at the Ru SA/GONa interface (b), highlighting the interfacial charge transfer characteristics. (c) Spatial representation of the HOMO and LUMO orbital distributions for the Ru SA/GONa configuration. Reproduced from Ref. [154] with permission. Copyright 2023, Elsevier.

Fig. 22. (a) Evolved gas amount during photocatalytic CO2 reduction. (b) Corresponding CO2 photoreduction rate. (c) Control experiments under various reaction conditions. (d) Cycling performance. (e) Stability evaluation. (f) Proposed reaction mechanism for CO2 photoreduction in the O/La-C3N4 system. Reproduced from Ref. [34] with permission. Copyright 2020, American Chemical Society. (g) Photocatalytic CO2 reduction activity of Cs3Bi2Br9 and Co-NG under varied conditions (presence or absence of light, catalyst, and CO2 atmosphere). (h) CO generation rates of Cs3Bi2Br9 and Cs3Bi2Br9/xCo-NG composites (x = 1, 3, 5, 7). (i) Cycling stability of Cs3Bi2Br9/5Co-NG over ten consecutive 4-h photocatalytic runs. Reproduced from Ref. [163] with permission. Copyright 2024, Elsevier.

Fig. 20. (a) Power-law decay fitting (ITAS∝(t-t0)-β) for bCN, Co-bCN, and IL/bCN under an N2/H2O vapor atmosphere, excited at 355 nm and monitored at 900 nm. (b) In-situ μsTAS spectra of IL/Co-bCN recorded in N2/H2O and CO2/H2O vapor environments under 355 nm excitation. (c) Correlation between electron transfer rates (ETRs) and ionic liquid loading on IL/bCN (black circles) and IL/Co-bCN (red squares), where rate constants are derived from the linear fit slope and background rates from the intercept. Reproduced from Ref. [77]. Copyright 2023, The Authors. Published by Springer Nature under the Creative Commons CC BY.

Fig. 23. (a) Comparison between the photocatalytic CO2 reduction performances of TiO2 and TiO2-Bi. (b) Variation in the amount of CO and CH4 during the 14 h-long test process. (c) Schematic of the CO2 reduction process. Reproduced from Ref. [166] with permission. Copyright 2018, Springer Nature. Photocatalytic CO2 reduction performance in acetonitrile aqueous solution. (d) Photocatalytic product evolution as a function of light irradiation times on Cu-Ti-Vo/Ti0.91O2-SL. Product formation rates (e) and electron-based selectivity (f) on Ti0.91O2-SL, Cu-O/Ti0.91O2-SL, and Cu-Ti-Vo/Ti0.91O2-SL. (Error bars indicate standard deviations.). Reproduced from Ref. [155]. Copyright 2023, The Author (s). Published by Springer Nature Licensed under CC BY. Performance of photocatalytic CO2 reduction. (g) Photocatalytic activity of the different catalysts. (h) Cycling tests of CH3COOH yield for 3%Cu/WO3, in which the error bars represent the standard deviations of five independent measurements. (i) Proposed PCR mechanism on the catalyst surface. Reproduced from Ref. [167] with permission. Copyright 2022, Elsevier.

Fig. 24. (a) Comparison of CO and H2 generation by nanosheet (CON) and bulk (COF) forms of Co-FPy-COF, Co-Py-COF, and Co-Bp-COF under visible light (λ > 420 nm, 300 W Xe lamp) using Ir[dF(CF3)ppy]2(dtbpy)PF6 as a photosensitizer. (b) CO turnover numbers for Co-FPy-CON versus molecular Co(Bpy) complexes under identical conditions. (c) 13CO detection from 13CO2 reduction using Co-FPy-CON, confirmed by mass spectrometry (inset: GC trace). (d) Recyclability of Co-FPy-CON shown via repeated CO and H2 evolution over multiple 2-h cycles with photosensitizer added after each run. Reproduced from Ref. [172] with permission. Copyright 2020, American Chemical Society. (e) Proposed photocatalytic CO2 reduction mechanism on the surface of Fe1/Ti3-xC?Ty MXene. Reproduced from Ref. [118] with permission. Copyright 2024, The Royal Society of Chemistry. (f) Comparative CO and H2 production profiles under different photocatalytic systems, highlighting the enhanced CO yield of the [Ru(bpy)3]Cl2/Te NS-ACS system. (g) Recyclability test over four consecutive cycles. (h) GC-MS analysis confirming 13CO as the product from 13CO2 reduction. (i) Schematic of the proposed CO2 photoreduction pathway over Te NS-ACS. Reproduced from Ref. [174] with permission. Copyright 2020, John Wiley and Sons.

Table 1 Summary of the photocatalytic CO2 reduction performance across various 2D supports anchored on single-atom catalysts.

2D support			SAC with loading wt%		Mode of reaction	Light source		Product yield (C₁ vs. C₂⁺) (μmol g⁻¹ h⁻¹)		Selectivity (%)		Quantum efficiency	Year of publication
Carbon-based	g-C₃N₄		La single atom (1.65 wt%)		solid-liquid (MeCN/H₂O + TEOA)	300 W Xe lamp (simulated solar light)		CO: 92 CH₄: 5.6 (C₁)		CO: 80.3		—	2020 [34]
	g-C₃N₄		Fe single atom + K⁺ (‒)		solid-liquid (0.075 mol L^-1 KOH solution)	300 W Xe lamp		CO: 20.00 CH₄: 0.32 (C₁)		CO: 100		2.86% (at 450 nm)	2022 [161]
	g-C₃N₄		Thulium (1 wt%)		solid-liquid (aqueous CO₂ suspension)	300 W Xe lamp (λ > 420 nm)		CO: 132.4 CH₄: 6.2 (C₁)		CO: 95.6		3.21% (at 420 nm)	2024 [162]
	g-C₃N₄		In^δ⁺-N₄ single atoms (‒)		gas-solid (no sacrificial agent)	300 W Xe lamp		CO: 398.87 (C₁)		CO ≈ 100		0.21% (AQE at 420 nm)	2023 [134]
	g-C₃N₄		Co (≈ 2.5 wt%)		solid-liquid (MeCN/H₂O + TEOA)	300 W Xe lamp (λ > 420 nm)		CO: 394.4 (C₁)		CO ≈ 81		—	2022 [160]
	porous g-C₃N₄ nanosheet		Pt (0.519 wt%)		gas-solid (H₂O vapor as reductant)	300 W Xe lamp		CO: 84.8; CH₄: ~0 (C₁)		CO ≈ 100		1.35% (at 400 nm)	2024 [72]
	crystalline g-C₃N₄ nanorods		Cu (‒)		gas-solid (CO₂ + H₂O vapor; no sacrificial agent)	300 W Xe lamp		CO: 3.086; CH₄: trace (C₁)		CO ≈ 100		—	2020 [32]
	ultrathin g-C₃N₄ nanosheets		Co (≈ 0.5 wt%)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (UV-vis)		CO: 40.5; CH₄: 6.3 (C₁)		100		AQY 1.00% @405 nm	2023 [77]
	g-C₃N₄		Pd (≈ 1.9 wt%)		Gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (λ > 385 nm)		CH₄: 20.3; CO: 0.8 (C₁)		CH₄:97.8		AQY 2.93% @385 nm	2022 [149]
	porous g-C₃N₄ nanosheets		Co (24.6 wt%)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp		CH₃OH: 235.5; CO: 2.9; CH₄: 3.4 (C₁); C₂H₄: 1.1; C₃H₆: 1.4; CH₃OCH₃: 3.3 (C₂)		CH₃OH ≈ 96.2		—	2022 [141]
	g-C₃N₄ nanosheets		Cu (0.24 wt%)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (1000 mW cm⁻²)		CO: 18.88 (C₁)		CO ≈ 100		AQE 0.0974% @365 nm; 0.0046% @420 nm	2024 [121]
	g-C₃N₄ nanosheets		Ni (≈ 0.7 wt%)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (UV-vis)		CO: 22.1; CH₄: 8.7 (C₁)		≈ 100		‒	2021 [33]
	g-C₃N₄ nanosheets		Sm (1.30 wt%)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (visible light, λ > 420 nm)		CO: 44.27 (C₁)		CO: 96.8		AQY 2.64% @420 nm	2025 [94]
	g-C₃N₄		Au (‒)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (visible light, λ > 420 nm)		CO: 8.68; CH₄: 0.96 (C₁)		—		—	2020 [99]
	g-C₃N₄		Fe (1.4 wt%)		solid-liquid suspension (CO₂in H₂O; no sacrificial agent/photosensitizer)	300 W Xe lamp		CO: 5.1 (C₁)		—		—	2021 [100]
	graphene		Co (‒)		gas-solid (CO₂ + H₂O vapor	300 W Xe lamp (200 mW cm⁻²)		CO: 123.16 (C₁)		CO: 100		—	2024 [163]
	partially oxidized graphene nanosheets		Co (‒)		homogeneous -heterogeneous hybrid system [Ru(bpy)₃]²⁺ as photosensitizer)	300 W Xe lamp (visible light, λ > 420 nm)		— (reported as TON = 678; TOF = 3.77 min^-1; CO only): (C₁)		CO: 100		—	2018 [31]
Metal oxide-based	TiO₂ nanosheets	Cu (‒)		Gas-solid (CO₂ + H₂O vapor; no sacrificial agent)		300 W Xe lamp	CO: 1.6 (C₁)		—		—		2019 [132]
	TiO₂ nanosheets	Bi (‒)		Gas-solid (CO₂ + H₂O)		300 W Xe lamp	CH₄: 10.94; CO: 0.46		—		—		2017 [166]
	Ti_0.91O₂single layer nanosheets	Cu (0.29 wt%)		Solid-liquid (CO₂-saturated acetonitrile: H₂O = 5:1)		300 W Xe lamp (λ > 420 nm)	CO: 18.6 (C₁); C₂H₄: 7.6; C₃H₈: 13.8 (C₂⁺)		C₃H₈: 64.88;86.2 (total C₂⁺)		QE: 0.48% @385 nm; 0.15% @415 nm; 0.06% @520 nm		2023 [155]
	h′-H_xWO₃nanosheets	Cu (3 wt%)		Solid-liquid (CO₂ + H₂O; no organic solvent)		300 W Xe lamp	CH₃COOH: 2.87 (C₂⁺)		CH₃COOH ≈ 67		—		2023 [167]
	ZrO₂ nanosheets	Ni (5 wt%)		Gas-solid (CO₂ + H₂O vapor; no solvent)		300 W Xe lamp (Light intensity: 5.0 W cm⁻²)	CO: 11.8 (C₁)		CO: 92.5		AQE 0.92% @365 nm; 0.36% @420 nm		2022 [106]
	CeO₂nanosheets	Pd (‒)		—		—	CH₄: 41.6 (C₁)		CH₄ ≈ 100		—		2022 [168]
	Nb₂O₅ nanosheets	Pd (1.54 wt%)		Gas-solid (CO₂+ H₂O vapor) reaction system		300 W xenon lamp (100 mW cm⁻²)	CO: 13.2; CH₄: 5.86 (C₁); CH₃COOH: 13.5; C₂H₄: 1.75 (C₂⁺)		—		AQY≈ 0.06% and 0.009% @350 nm		2025 [169]
	Amorphous In₂O₃ nanosheets	Cu (~12.2 atom %)		Gas-solid (CO₂ + H₂O vapor; no sacrificial agent)		300 W Xe lamp (full spectrum)	C₂H₆O: 798.7 (C₂⁺); CH₄: 4.1 (C₁)		C₂H₆O: 99.5		0.17% (ethanol)		2023 [170]
	CO₃O₄	Pd (‒)		Gas-solid (CO₂ + H₂O vapor; no sacrificial agent)		300 W xenon lamp (100 mW cm⁻²)	CH₃COOH: 13.4 (C₂⁺)		CH₃COOH≈100		—		2024 [120]
Emerging-based	COF	Mo (‒)		Gas-solid (CO₂ + H₂O vapor; no sacrificial agent)		300 W Xe lamp (λ ≥ 420 nm)	CO: 6.19; CH₄: 1.08 (C₁); C₂H₄: 3.57 (C₂⁺)		CO: 57.12; CH₄: 9.96; C₂H₄: 32.92		—		2021 [171]
	COF nanosheets	Co (2.1 wt%)		Liquid-phase		300 W Xe lamp (λ > 420 nm)	CO: 1.68 (C₁)		CO: 76		6.6% @420 nm		2020 [172]
	MOF nanosheets	Co (6.0 wt%)		Liquid-phase (aqueous, with [Ru(bpy)₃]Cl₂ photosensitizer and ascorbic acid sacrificial agent)		300 W Xe lamp (λ > 420 nm)	CO: 7041 (C₁)		CO: 86		—		2023 [173]
	Ti_3-xC₂T_y MXene nanosheets	Fe (3.7 wt%)		Gas-solid (CO₂ + H₂O vapor; no sacrificial agent)		300 W Xe lamp	CO: 259.0; CH₄: 38.8 (C₁)		—		—		2024 [118]
	Bi₃O₄Br	Co (1 wt%)		Gas-solid (CO₂ + H₂O; no sacrificial agent or photosensitizer)		300 W Xe lamp	CO: 107.1 (C₁)		—		—		2019 [92]
	BP nanosheets	Co		Liquid-phase ([Ru(bpy)₃]²⁺photosensitizer)		300 W Xe lamp	CO: 88.6 (C₁)		CO: 59.2		—		2020 [130]
	Te nanosheets	Co		Gas-solid ([Ru(bpy)₃]Cl₂ as the photosensitizer)		300 W Xe lamp (λ > 420 nm)	CO: 52.3 (C₁)		—		—		2020 [174]

Table 1 Summary of the photocatalytic CO2 reduction performance across various 2D supports anchored on single-atom catalysts.

2D support			SAC with loading wt%		Mode of reaction	Light source		Product yield (C₁ vs. C₂⁺) (μmol g⁻¹ h⁻¹)		Selectivity (%)		Quantum efficiency	Year of publication
Carbon-based	g-C₃N₄		La single atom (1.65 wt%)		solid-liquid (MeCN/H₂O + TEOA)	300 W Xe lamp (simulated solar light)		CO: 92 CH₄: 5.6 (C₁)		CO: 80.3		—	2020 [34]
	g-C₃N₄		Fe single atom + K⁺ (‒)		solid-liquid (0.075 mol L^-1 KOH solution)	300 W Xe lamp		CO: 20.00 CH₄: 0.32 (C₁)		CO: 100		2.86% (at 450 nm)	2022 [161]
	g-C₃N₄		Thulium (1 wt%)		solid-liquid (aqueous CO₂ suspension)	300 W Xe lamp (λ > 420 nm)		CO: 132.4 CH₄: 6.2 (C₁)		CO: 95.6		3.21% (at 420 nm)	2024 [162]
	g-C₃N₄		In^δ⁺-N₄ single atoms (‒)		gas-solid (no sacrificial agent)	300 W Xe lamp		CO: 398.87 (C₁)		CO ≈ 100		0.21% (AQE at 420 nm)	2023 [134]
	g-C₃N₄		Co (≈ 2.5 wt%)		solid-liquid (MeCN/H₂O + TEOA)	300 W Xe lamp (λ > 420 nm)		CO: 394.4 (C₁)		CO ≈ 81		—	2022 [160]
	porous g-C₃N₄ nanosheet		Pt (0.519 wt%)		gas-solid (H₂O vapor as reductant)	300 W Xe lamp		CO: 84.8; CH₄: ~0 (C₁)		CO ≈ 100		1.35% (at 400 nm)	2024 [72]
	crystalline g-C₃N₄ nanorods		Cu (‒)		gas-solid (CO₂ + H₂O vapor; no sacrificial agent)	300 W Xe lamp		CO: 3.086; CH₄: trace (C₁)		CO ≈ 100		—	2020 [32]
	ultrathin g-C₃N₄ nanosheets		Co (≈ 0.5 wt%)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (UV-vis)		CO: 40.5; CH₄: 6.3 (C₁)		100		AQY 1.00% @405 nm	2023 [77]
	g-C₃N₄		Pd (≈ 1.9 wt%)		Gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (λ > 385 nm)		CH₄: 20.3; CO: 0.8 (C₁)		CH₄:97.8		AQY 2.93% @385 nm	2022 [149]
	porous g-C₃N₄ nanosheets		Co (24.6 wt%)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp		CH₃OH: 235.5; CO: 2.9; CH₄: 3.4 (C₁); C₂H₄: 1.1; C₃H₆: 1.4; CH₃OCH₃: 3.3 (C₂)		CH₃OH ≈ 96.2		—	2022 [141]
	g-C₃N₄ nanosheets		Cu (0.24 wt%)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (1000 mW cm⁻²)		CO: 18.88 (C₁)		CO ≈ 100		AQE 0.0974% @365 nm; 0.0046% @420 nm	2024 [121]
	g-C₃N₄ nanosheets		Ni (≈ 0.7 wt%)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (UV-vis)		CO: 22.1; CH₄: 8.7 (C₁)		≈ 100		‒	2021 [33]
	g-C₃N₄ nanosheets		Sm (1.30 wt%)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (visible light, λ > 420 nm)		CO: 44.27 (C₁)		CO: 96.8		AQY 2.64% @420 nm	2025 [94]
	g-C₃N₄		Au (‒)		gas-solid (CO₂ + H₂O vapor, no sacrificial agent)	300 W Xe lamp (visible light, λ > 420 nm)		CO: 8.68; CH₄: 0.96 (C₁)		—		—	2020 [99]
	g-C₃N₄		Fe (1.4 wt%)		solid-liquid suspension (CO₂in H₂O; no sacrificial agent/photosensitizer)	300 W Xe lamp		CO: 5.1 (C₁)		—		—	2021 [100]
	graphene		Co (‒)		gas-solid (CO₂ + H₂O vapor	300 W Xe lamp (200 mW cm⁻²)		CO: 123.16 (C₁)		CO: 100		—	2024 [163]
	partially oxidized graphene nanosheets		Co (‒)		homogeneous -heterogeneous hybrid system [Ru(bpy)₃]²⁺ as photosensitizer)	300 W Xe lamp (visible light, λ > 420 nm)		— (reported as TON = 678; TOF = 3.77 min^-1; CO only): (C₁)		CO: 100		—	2018 [31]
Metal oxide-based	TiO₂ nanosheets	Cu (‒)		Gas-solid (CO₂ + H₂O vapor; no sacrificial agent)		300 W Xe lamp	CO: 1.6 (C₁)		—		—		2019 [132]
	TiO₂ nanosheets	Bi (‒)		Gas-solid (CO₂ + H₂O)		300 W Xe lamp	CH₄: 10.94; CO: 0.46		—		—		2017 [166]
	Ti_0.91O₂single layer nanosheets	Cu (0.29 wt%)		Solid-liquid (CO₂-saturated acetonitrile: H₂O = 5:1)		300 W Xe lamp (λ > 420 nm)	CO: 18.6 (C₁); C₂H₄: 7.6; C₃H₈: 13.8 (C₂⁺)		C₃H₈: 64.88;86.2 (total C₂⁺)		QE: 0.48% @385 nm; 0.15% @415 nm; 0.06% @520 nm		2023 [155]
	h′-H_xWO₃nanosheets	Cu (3 wt%)		Solid-liquid (CO₂ + H₂O; no organic solvent)		300 W Xe lamp	CH₃COOH: 2.87 (C₂⁺)		CH₃COOH ≈ 67		—		2023 [167]
	ZrO₂ nanosheets	Ni (5 wt%)		Gas-solid (CO₂ + H₂O vapor; no solvent)		300 W Xe lamp (Light intensity: 5.0 W cm⁻²)	CO: 11.8 (C₁)		CO: 92.5		AQE 0.92% @365 nm; 0.36% @420 nm		2022 [106]
	CeO₂nanosheets	Pd (‒)		—		—	CH₄: 41.6 (C₁)		CH₄ ≈ 100		—		2022 [168]
	Nb₂O₅ nanosheets	Pd (1.54 wt%)		Gas-solid (CO₂+ H₂O vapor) reaction system		300 W xenon lamp (100 mW cm⁻²)	CO: 13.2; CH₄: 5.86 (C₁); CH₃COOH: 13.5; C₂H₄: 1.75 (C₂⁺)		—		AQY≈ 0.06% and 0.009% @350 nm		2025 [169]
	Amorphous In₂O₃ nanosheets	Cu (~12.2 atom %)		Gas-solid (CO₂ + H₂O vapor; no sacrificial agent)		300 W Xe lamp (full spectrum)	C₂H₆O: 798.7 (C₂⁺); CH₄: 4.1 (C₁)		C₂H₆O: 99.5		0.17% (ethanol)		2023 [170]
	CO₃O₄	Pd (‒)		Gas-solid (CO₂ + H₂O vapor; no sacrificial agent)		300 W xenon lamp (100 mW cm⁻²)	CH₃COOH: 13.4 (C₂⁺)		CH₃COOH≈100		—		2024 [120]
Emerging-based	COF	Mo (‒)		Gas-solid (CO₂ + H₂O vapor; no sacrificial agent)		300 W Xe lamp (λ ≥ 420 nm)	CO: 6.19; CH₄: 1.08 (C₁); C₂H₄: 3.57 (C₂⁺)		CO: 57.12; CH₄: 9.96; C₂H₄: 32.92		—		2021 [171]
	COF nanosheets	Co (2.1 wt%)		Liquid-phase		300 W Xe lamp (λ > 420 nm)	CO: 1.68 (C₁)		CO: 76		6.6% @420 nm		2020 [172]
	MOF nanosheets	Co (6.0 wt%)		Liquid-phase (aqueous, with [Ru(bpy)₃]Cl₂ photosensitizer and ascorbic acid sacrificial agent)		300 W Xe lamp (λ > 420 nm)	CO: 7041 (C₁)		CO: 86		—		2023 [173]
	Ti_3-xC₂T_y MXene nanosheets	Fe (3.7 wt%)		Gas-solid (CO₂ + H₂O vapor; no sacrificial agent)		300 W Xe lamp	CO: 259.0; CH₄: 38.8 (C₁)		—		—		2024 [118]
	Bi₃O₄Br	Co (1 wt%)		Gas-solid (CO₂ + H₂O; no sacrificial agent or photosensitizer)		300 W Xe lamp	CO: 107.1 (C₁)		—		—		2019 [92]
	BP nanosheets	Co		Liquid-phase ([Ru(bpy)₃]²⁺photosensitizer)		300 W Xe lamp	CO: 88.6 (C₁)		CO: 59.2		—		2020 [130]
	Te nanosheets	Co		Gas-solid ([Ru(bpy)₃]Cl₂ as the photosensitizer)		300 W Xe lamp (λ > 420 nm)	CO: 52.3 (C₁)		—		—		2020 [174]

Fig. 25. Overview of challenges and engineering strategies for SAC/2D in photocatalytic CO2 reduction.

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二维(2D)材料上的单原子催化剂用于光催化CO₂还原: 基础、设计与新兴策略

Single-atom catalysts on two-dimensional (2D) materials for photocatalytic CO₂ reduction: Fundamentals, design, and emerging strategies

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