设计热力学稳定的贵金属单原子光催化剂用于乙醇的高效非氧化转化形成高纯氢和增值产物乙醛

引用本文: 周昱晨, 刘焕敏, 李红星, 宋欣妤, 唐永华, 周鹏. 设计热力学稳定的贵金属单原子光催化剂用于乙醇的高效非氧化转化形成高纯氢和增值产物乙醛[J]. 物理化学学报, 2025, 41(6): 100067. doi: 10.1016/j.actphy.2025.100067 shu

Citation: Yuchen Zhou, Huanmin Liu, Hongxing Li, Xinyu Song, Yonghua Tang, Peng Zhou. Designing thermodynamically stable noble metal single-atom photocatalysts for highly efficient non-oxidative conversion of ethanol into high-purity hydrogen and value-added acetaldehyde[J]. Acta Physico-Chimica Sinica, 2025, 41(6): 100067. doi: 10.1016/j.actphy.2025.100067 shu

设计热力学稳定的贵金属单原子光催化剂用于乙醇的高效非氧化转化形成高纯氢和增值产物乙醛

1.
北京大学深圳研究生院, 环境与能源学院, 生态环境与资源效率研究实验室, 广东深圳 518055;
2.
湘潭大学, 物理与光电工程学院, 湖南湘潭 411105
基金项目:
北京大学深圳研究生院启动基金和国家自然科学基金优秀青年科学家项目资助,同时感谢曙光超级计算机中心对本文计算的支持

摘要: 光催化剂固有的表面原子构型，通常缺乏不稳定或难以生成的原子空位，这往往限制了金属单原子(MSA)助催化剂与光催化剂之间有效相互作用的形成，从而抑制了单原子光催化剂的稳定性和性能提升。在本研究中，我们提出了一种简便且经济的光化学氧还原反应(ORR)机制，用于在温和条件下(仅消耗水和氧气，压力为101325 Pa，温度为25 °C)在TiO₂光催化剂上制备热力学稳定的贵金属单原子助催化剂。第一性原理模拟首次从理论上揭示了TiO₂的固有表面构型仅能产生不稳定的Pt―O₂结构。然而，TiO₂上发生的ORR不仅能够提供一个外来氧与Pt单原子(PtSA)配位，还能诱导一个表面晶格氧向PtSA移动，从而促进热力学稳定的Pt―O₄物种的形成，这一点通过在氧气氛围而非惰性氛围中实验合成TiO₂上的PtSA得到了验证。所获得的稳定PtSA-TiO₂光催化剂在共生产高纯度氢气和附加值乙醛时，表现出320.4 mmol·g^-1·h^-1的光催化速率，选择性高达99.65%，其活性是负载Pt纳米颗粒的TiO₂的三倍。该策略进一步扩展至其他贵金属，如Rh和Pd。

关键词:

English

Designing thermodynamically stable noble metal single-atom photocatalysts for highly efficient non-oxidative conversion of ethanol into high-purity hydrogen and value-added acetaldehyde

1.
Eco-environment and Resource Efficiency Research Laboratory, School of Environment and Energy, Peking University Shenzhen Graduate School, Shenzhen 518055, Guangdong Province, China;
2.
School of Physics and Optoelectronics, Xiangtan University, Xiangtan 411105, Hunan Province, China
Received Date: 18 January 2025
Accepted Date: 17 February 2025
Revised Date: 16 February 2025
Fund Project:
The project was supported by the start-up support from Peking University Shenzhen Graduate School and the National Natural Science Foundation Excellent Young Scientist Project, PKUSZ, China. The authors would like to thank the calculation support from Shuguang Supercomputer Center.

Abstract: The intrinsic surface atomic configuration of photocatalyst without unstable or difficult-to-generate atomic vacancies often limits the formation of effective interaction between metal single atom (MSA) cocatalyst and photocatalyst, thus inhibiting the stability and performance improvement of single-atom photocatalysts. In this study, we present a convenient and cost-effective photochemical oxygen reduction reaction (ORR) mechanism to prepare thermodynamically stable noble metal single-atom cocatalysts on TiO₂ photocatalyst under mild condition (only consuming water and oxygen at 101325 Pa and 25 °C). The first-principles simulation firstly theoretically reveals that the intrinsic surface configuration of TiO₂ can only produce unstable Pt―O₂ structure. However, ORR occurring on TiO₂ can not only provide one foreign oxygen to coordinate with Pt single atom (PtSA), but also induce one surface lattice oxygen to move toward PtSA, promoting the formation of one thermodynamically stable Pt―O₄ species, demonstrated by the experimental synthesis of PtSA on TiO₂ in oxygen atmosphere instead of inert atmosphere. The obtained stable PtSA-TiO₂ photocatalysts exhibit a photocatalytic rate of 320.4 mmol·g^-1·h^-1 for the coproduction of high-purity hydrogen and value-added acetaldehyde with a selectivity of 99.65%, three-fold higher than the activity of Pt nanoparticles-loaded TiO₂. This strategy is further extended to other noble metals, such as Rh and Pd.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

设计热力学稳定的贵金属单原子光催化剂用于乙醇的高效非氧化转化形成高纯氢和增值产物乙醛

English

Designing thermodynamically stable noble metal single-atom photocatalysts for highly efficient non-oxidative conversion of ethanol into high-purity hydrogen and value-added acetaldehyde

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设计热力学稳定的贵金属单原子光催化剂用于乙醇的高效非氧化转化形成高纯氢和增值产物乙醛

English

Designing thermodynamically stable noble metal single-atom photocatalysts for highly efficient non-oxidative conversion of ethanol into high-purity hydrogen and value-added acetaldehyde

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CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

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中国化学会秘书处

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs