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用于太阳能海水分解的原子分散在NC@Cu核壳结构上的钴

Atomic Dispersed Co on NC@Cu Core-Shells for Solar Seawater Splitting.

作者信息

Sun Zhehao, Cheng Shuwen, Jing Xuechen, Liu Kaili, Chen Yi-Lun, Wibowo Ary Anggara, Yin Hang, Usman Muhammad, MacDonald Daniel, Cheong Soshan, Webster Richard F, Gloag Lucy, Cox Nicholas, Tilley Richard D, Yin Zongyou

机构信息

Research School of Chemistry, The Australian National University, Canberra, Australian Capital Territory, 2601, Australia.

School of Engineering, The Australian National University, Canberra, Australian Capital Territory, 2601, Australia.

出版信息

Adv Mater. 2024 Dec;36(49):e2406088. doi: 10.1002/adma.202406088. Epub 2024 Oct 14.

DOI:10.1002/adma.202406088
PMID:39402768
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11619220/
Abstract

With freshwater resources becoming increasingly scarce, the photocatalytic seawater splitting for hydrogen production has garnered widespread attention. In this study, a novel photocatalyst consisting of a Cu core coated is introduced with N-doped C and decorated with single Co atoms (Co-NC@Cu) for solar to hydrogen production from seawater. This catalyst, without using noble metals or sacrificial agents, demonstrates superior hydrogen production effficiency of 9080 µmolgh, i.e., 4.78% solar-to-hydrogen conversion efficiency, and exceptional long-term stability, operating over 340 h continuously. The superior performance is attributed to several key factors. First, the focus-light induced photothermal effect enhances redox reaction capabilities, while the salt-ions enabled charge polarization around catalyst surfaces extends charge carrier lifetime. Furthermore, the Co─NC@Cu exhibits excellent broad light absorption, promoting photoexcited charge production. Theoretical calculations reveal that Co─NC acts as the active site, showing low energy barriers for reduction reactions. Additionally, the formation of a strong surface electric field from the localized surface plasmon resonance (LSPR) of Cu nanoparticles further reduces energy barriers for redox reactions, improving seawater splitting activity. This work provides valuable insights into intergrating the reaction environment, broad solar absorption, LSPR, and active single atoms into a core-shell photocatalyst design for efficient and robust solar-driven seawater splitting.

摘要

随着淡水资源日益稀缺,光催化海水分解制氢受到了广泛关注。在本研究中,引入了一种新型光催化剂,它由包覆有氮掺杂碳的铜核组成,并装饰有单钴原子(Co-NC@Cu),用于海水太阳能制氢。这种催化剂无需使用贵金属或牺牲剂,展现出9080 μmol g h的卓越产氢效率,即太阳能到氢能的转换效率为4.78%,并且具有出色的长期稳定性,可连续运行超过340小时。其卓越性能归因于几个关键因素。首先,聚焦光诱导的光热效应增强了氧化还原反应能力,而盐离子在催化剂表面实现的电荷极化延长了电荷载流子寿命。此外,Co-NC@Cu表现出优异的宽光谱光吸收,促进了光生电荷的产生。理论计算表明,Co-NC作为活性位点,还原反应的能垒较低。此外,铜纳米颗粒的局域表面等离子体共振(LSPR)形成的强表面电场进一步降低了氧化还原反应的能垒,提高了海水分解活性。这项工作为将反应环境、宽光谱太阳能吸收、LSPR和活性单原子整合到核壳光催化剂设计中以实现高效且稳定的太阳能驱动海水分解提供了有价值的见解。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b782/11619220/c88adf3da5d1/ADMA-36-2406088-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b782/11619220/68ca86931d4b/ADMA-36-2406088-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b782/11619220/baac56b49618/ADMA-36-2406088-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b782/11619220/bf1a59622a4a/ADMA-36-2406088-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b782/11619220/be37f67903f9/ADMA-36-2406088-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b782/11619220/c88adf3da5d1/ADMA-36-2406088-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b782/11619220/68ca86931d4b/ADMA-36-2406088-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b782/11619220/baac56b49618/ADMA-36-2406088-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b782/11619220/bf1a59622a4a/ADMA-36-2406088-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b782/11619220/be37f67903f9/ADMA-36-2406088-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b782/11619220/c88adf3da5d1/ADMA-36-2406088-g002.jpg

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Continuous electroproduction of formate via CO reduction on local symmetry-broken single-atom catalysts.通过在局部对称性破缺的单原子催化剂上进行CO还原连续电生产甲酸盐。
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Confined Heterojunction in Hollow-Structured TiO and Its Directed Effect in Photodriven Seawater Splitting.
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