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用于太阳能制氢及原位光化学合成铂单原子修饰硫化镉纳米颗粒的镉/铂前驱体溶液

Cd/Pt Precursor Solution for Solar H Production and in situ Photochemical Synthesis of Pt Single-atom Decorated CdS Nanoparticles.

作者信息

Sharma Pankaj, Sharma Monika, Dearg Malcolm, Wilding Martin, Slater Thomas J A, Catlow C Richard A

机构信息

School of Chemistry, Cardiff University, Cardiff, CF10 3AT, UK.

UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell, OX11 0FA, UK.

出版信息

Angew Chem Int Ed Engl. 2023 May 8;62(20):e202301239. doi: 10.1002/anie.202301239. Epub 2023 Mar 10.

DOI:10.1002/anie.202301239
PMID:36788107
Abstract

Despite extensive efforts to develop high-performance H evolution catalysts, this remains a major challenge. Here, we demonstrate the use of Cd/Pt precursor solutions for significant photocatalytic H production (154.7 mmol g  h ), removing the need for a pre-synthesized photocatalyst. In addition, we also report simultaneous in situ synthesis of Pt single-atoms anchored CdS nanoparticles (Pt -CdS ) during photoirradiation. The highly dispersed in situ incorporation of extensive Pt single atoms on CdS enables the enhancement of active sites and suppresses charge recombination, which results in exceptionally high solar-to-hydrogen conversion efficiency of ≈1 % and an apparent quantum yield of over 91 % (365 nm) for H production. Our work not only provides a promising strategy for maximising H production efficiency but also provides a green process for H production and the synthesis of highly photoactive Pt -CdS nanoparticles.

摘要

尽管人们为开发高性能析氢催化剂付出了巨大努力,但这仍然是一个重大挑战。在此,我们展示了使用镉/铂前驱体溶液实现显著的光催化析氢(154.7 mmol g⁻¹ h⁻¹),无需预先合成光催化剂。此外,我们还报道了在光辐照过程中同时原位合成铂单原子锚定的硫化镉纳米颗粒(Pt₁-CdS)。大量铂单原子高度分散地原位掺入硫化镉中,能够增加活性位点并抑制电荷复合,这导致了高达约1%的卓越太阳能到氢能转换效率以及超过91%(365 nm)的析氢表观量子产率。我们的工作不仅为最大化析氢效率提供了一种有前景的策略,还为析氢以及高光活性Pt₁-CdS纳米颗粒的合成提供了一个绿色过程。

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