连续单电子氧还原增强的S型SbVO4/PCN异质结在环境条件下高效人工光合成双氧水

doi:10.1016/S1872-2067(26)65203-5

催化学报 ›› 2026, Vol. 91: 241-251.DOI: 10.1016/S1872-2067(26)65203-5

连续单电子氧还原增强的S型SbVO₄/PCN异质结在环境条件下高效人工光合成双氧水

王壮壮^a, 李源^a, 程强^a, 王小田^a, 刘彬^b^,^c, 张高科^a^,^*()

^a 武汉理工大学资源与环境工程学院, 湖北武汉 430070
^b 香港城市大学材料科学与工程系, 香港 999077
^c 香港城市大学化学系及超金刚石与先进薄膜研究中心, 香港 999077

收稿日期:2025-12-18 接受日期:2026-02-04 出版日期:2026-12-18 发布日期:2026-10-13
通讯作者: ^*电子信箱: gkzhang@whut.edu.cn (张高科).
基金资助:
国家自然科学基金(22176151);国家自然科学基金(92163125);国家自然科学基金(22361132537);香港城市大学科研启动基金(9020003);创新科技署研究人才库-全球科学、技术、工程和数学教授计划(9446006)

Boosting sequential single-electron O₂ reduction reaction on S-scheme SbVO₄/PCN heterojunction for efficient artificial photosynthesis of H₂O₂ under ambient condition

Zhuangzhuang Wang^a, Yuan Li^a, Qiang Cheng^a, Xiaotian Wang^a, Bin Liu^b^,^c, Gaoke Zhang^a^,^*()

^a School of Resources and Environmental Engineering, Wuhan University of Technology, Wuhan 430070, Hubei, China
^b Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, Hongkong SAR 999077, China
^c Department of Chemistry & Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Kowloon, Hongkong SAR 999077, China

Received:2025-12-18 Accepted:2026-02-04 Online:2026-12-18 Published:2026-10-13
Supported by:
National Natural Science Foundation of China(22176151);National Natural Science Foundation of China(92163125);National Natural Science Foundation of China(22361132537);City University of Hong Kong Startup fund(9020003);ITF-RTH-Global Stem Professorship(9446006)

摘要/Abstract

摘要：

过氧化氢(H₂O₂)是应用极为广泛的大宗基础化工产品. 当前工业主流的蒽醌法生产H₂O₂存在能耗高、工艺流程复杂以及伴生有毒副产物等弊端, 严重制约了过氧化氢产业的绿色可持续发展. 基于光催化反应技术的人工光合成H₂O₂, 被视作极具前景的环境友好型替代技术. 在诸多光催化反应路径中, 分步单电子氧还原反应(SSORR)凭借较低的热力学势垒, 成为人工光合成H₂O₂的重要研究方向. 然而, 该反应过程普遍受限于氧气补给不足, *O₂向*OOH中间体转化效率低以及光生载流子复合过快等动力学瓶颈, 致使H₂O₂生成速率偏低. 因此, 构建增强光生载流子分离, 促进氧分子活化, 且能原位供给反应物的光催化体系, 实现H₂O₂的高效合成, 对推动人工光合成H₂O₂技术的发展具有重要的科学意义.
针对光催化合成H₂O₂过程中存在的诸多关键科学问题, 本研究通过简便的水热原位生长策略, 将SbVO₄纳米颗粒均匀负载于PCN(聚合氮化碳)表面, 制备了一种界面结合紧密的S型SbVO₄/PCN复合异质结光催化剂, 旨在纯水体系和常温常压条件下实现无牺牲剂的人工光合成H₂O₂. 光催化性能测试表明, 最优样品10-SbVO₄/PCN在可见光(λ > 420 nm)照射下, H₂O₂生成速率高达94.7 μmol·g^-1·h^-1, 为纯PCN样品的41倍, 且在长时间反应过程中展现出优异的结构稳定性与催化性能稳定性. 更重要的是, 该体系在365和420 nm单色光光照条件下, 太阳能-化学能转换效率分别可达0.38%和0.34%, 表观量子效率分别为4.1%和3.5%. 原位漫反射红外光谱检测结果表明, 人工光合成H₂O₂反应过程中存在*O₂^-和*OOH等关键中间体, 证实了该反应中H₂O₂的生成遵循SSORR反应路径, 即O₂ + e^- → ·O₂^-, O₂ + H⁺ + e^- → ·OOH, OOH + H⁺ + e^-→ H₂O₂的分步反应路径, 而非直接两电子氧还原过程. 光催化机理研究表明, SbVO₄与PCN之间的功函数差异诱导形成内建电场, 在光照条件下, SbVO₄导带中的光生电子会定向转移至PCN价带, 与PCN价带中的光生空穴复合, 保留了PCN导带中具有高还原电位的电子用于SSORR反应, 以及SbVO₄价带中具有高氧化电位的空穴用于水氧化反应. 密度泛函理论计算进一步证实, SbVO₄/PCN异质结内杂化p轨道电子倾向于转移至O₂的1π与2π*轨道, 显著削弱了O₂分子中的O=O键, 致使*O₂向*OOH的转化呈现热力学自发特征, 进而有效降低了SSORR路径的反应能垒. 同时, SbVO₄表面发生的水氧化反应可原位持续生成O₂和H⁺, 自发补充SSORR反应所需的反应物, 极大地提升了整体反应的动力学性能, 最终实现了H₂O₂的高效光催化合成.
综上，本研究通过构建多效增强的S型SbVO₄/PCN异质结光催化剂, 成功解决了光催化合成H₂O₂过程中存在的反应物补给不足, 中间产物转化效率低, 光生载流子复合过快的三大动力学瓶颈, 为常温常压且无牺牲剂条件下高效光合成H₂O₂提供了新的材料设计思路, 也进一步拓展了S型光催化体系的研究方向.

关键词: 人工光合成, 连续单电子氧还原, H₂O₂, S型异质结, SbVO₄/PCN

Abstract:

Non-sacrificial artificial photosynthesis of H₂O₂ offers a charming process for onsite H₂O₂ generation with unique merits of sustainability and environmental friendliness. However, the low conversion efficiency of sequential single-electron oxygen reduction reaction (SSORR) greatly limits the H₂O₂ production rate. Herein, we develop a step-scheme (S-scheme) SbVO₄/PCN system for artificial photosynthesis of H₂O₂, which displays greatly boosted photocatalytic SSORR. The H₂O₂ yield can reach as high as 94.7 μmol·g-catalyst^-1·h^-1 under visible light illumination (λ > 420 nm), about 41 times higher than that of the pristine PCN. The S-scheme charge transfer pathway is systematically demonstrated by photo-irradiated Kelvin probe force microscopy, in-situ X-ray photoelectron spectroscopy and surface photovoltage measurements. Theoretical calculations further indicate that the SbVO₄/PCN is favorable to transfer electrons from its hybrid p orbitals to the 1π and 2π* orbitals of O₂ and the evolution from *O₂ to *OOH consumes no energy, therefore greatly promoting the formation of PCN-*OOH even without electron donor. The onsite generated O₂ via water oxidation reaction on SbVO₄ can replenish its consumption on PCN, leading to boosted reaction kinetics.

Key words: Artificial photosynthesis, Sequential single-electron oxygen reduction reaction, H₂O₂, S-scheme, SbVO₄/PCN

王壮壮, 李源, 程强, 王小田, 刘彬, 张高科. 连续单电子氧还原增强的S型SbVO₄/PCN异质结在环境条件下高效人工光合成双氧水[J]. 催化学报, 2026, 91: 241-251.

Zhuangzhuang Wang, Yuan Li, Qiang Cheng, Xiaotian Wang, Bin Liu, Gaoke Zhang. Boosting sequential single-electron O₂ reduction reaction on S-scheme SbVO₄/PCN heterojunction for efficient artificial photosynthesis of H₂O₂ under ambient condition[J]. Chinese Journal of Catalysis, 2026, 91: 241-251.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65203-5

https://www.cjcatal.com/CN/Y2026/V91/I12/241

图/表 5

Fig. 1. (a) Schematic illustration showing the synthetic process of 10-SbV/PCN nanocomposites. (b,c) TEM images of 10-SbV/PCN nanocomposites. (d) HRTEM image of 10-SbV/PCN nanocomposites. (e) EDS elemental mapping images of 10-SbV/PCN nanocomposites.

Fig. 2. (a) Long-term photocatalytic H2O2 production catalyzed by pristine PCN (pink color) and 10-SbV/PCN (yellow color) under different irradiation wavelength. (b) Solar-to-chemical conversion efficiency of 10-SbV/PCN under 365 and 420 nm light irradiation in pure water and open air. (c) Apparent quantum yield of 10-SbV/PCN under 365 and 420 nm light irradiation in pure water and open air. (d) In-situ DRIFTS spectra recorded over 10-SbV/PCN. Photocatalytic O2 (e) and H2 (f) evolution over PCN and 10-SbV/PCN.

Fig. 3. (a) In-situ and ex-situ survey XPS spectra of different catalysts. In-situ and ex-situ high-resolution XPS spectra of C 1s (b), N 1s (c), V 3d (d), Sb 3d (e), and O 1s (f). In-situ XPS spectra were collected under the irradiation of 365 nm light.

Fig. 4. Surface potential distribution of 10-SbV/PCN in dark (a) and under 365 nm light irradiation (b). (c) The line-scanning surface potential from A1 to B1 in dark and A2 to B2 under 365 nm light irradiation, respectively. (d) Surface photovoltage spectra of pristine PCN and 10-SbV/PCN. (e) Surface photocurrent spectra of PCN and 10-SbV/PCN. (f) TRPL spectra of PCN and 10-SbV/PCN.

Fig. 5. The calculated electrostatic potential of (111) plane of SbV (a) and its corresponding structural model along the [111] direction (b). The calculated electrostatic potential of (001) plane of PCN (c) and its corresponding structural model along the [001] direction (d). The planar-averaged electron density difference Δρ (e) and the side-view of the charge density difference (f) over the SbV/PCN heterojunction. Inset shows the electronic location function of SbV/PCN (the red and green colors represent electron accumulation and depletion, respectively). (g) The interaction of px+py orbitals of SbV/PCN and O2 orbitals after O2 adsorption on SbV/PCN. (h) Free energy of sequential single-electron ORR. (i) Proposed photocatalytic mechanism of SbV/PCN heterojunction for robust production of H2O2.

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连续单电子氧还原增强的S型SbVO₄/PCN异质结在环境条件下高效人工光合成双氧水

Boosting sequential single-electron O₂ reduction reaction on S-scheme SbVO₄/PCN heterojunction for efficient artificial photosynthesis of H₂O₂ under ambient condition

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