Water Splitting Using a Photocatalyst with Single-Atom Reaction Sites
Water Splitting Using a Photocatalyst with Single-Atom Reaction Sites
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DOI：
10.1021/acs.jpcc.0c03132
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发表时间：
2020-09-24
影响因子：
3.7
通讯作者：
Ida, Shintaro
中科院分区：
文献类型：
--
作者：
Hsu, Chu-Wei;Awaya, Keisuke;Ida, Shintaro
掺杂分离的单原子析氢反应位点的纳米片是抑制光催化水分解过程中重组的一种潜在手段。在晶格中掺杂单原子反应位点后，氧化纳米片在CH3OH/水的光催化析氢过程中表现出更高的活性。然而，水从纯水分解成H-2和O-2还没有在这些材料上实现，因为逆向反应，如氧还原，也在这些相同的反应位点加速。在本研究中，制备了含有Rh单原子反应位点的铌酸钙纳米片，并覆盖了超薄的NiOx原子层。发现Ni/Rh原子比为7/1的纳米片促进了H-2和O-2从水中的演化。在该体系中，超薄的NiOx原子层阻止了氧的渗透，但允许H+进入Rh反应位点，从而促进光催化水裂解生成H-2和O2。这是首次使用单原子反应位点的纳米片光催化剂实现完美的水分解。
Nanosheets doped with isolated single-atom reaction sites for hydrogen evolution are a potential means of suppressing recombination during photocatalytic water splitting. Oxide nanosheets show higher activity during photocatalytic hydrogen evolution from CH3OH/water after doping with single-atom reaction sites in the lattice. However, water splitting into H-2 and O-2 from pure water has not yet been achieved on such materials because backward reactions, such as oxygen reduction, are also accelerated at these same reaction sites. In the present study, calcium niobate nanosheets incorporating Rh single-atom reaction sites covered with ultrathin NiOx atomic layers are fabricated. The nanosheets having a Ni/Rh atomic ratio of 7/1 are found to promote evolution of H-2 and O-2 from water. In this system, the ultrathin NiOx atomic layers prevent oxygen penetration but allow H+ to access the Rh reaction sites, thus promoting photocatalytic water splitting for H-2 and O2 production. This is the first demonstration of perfect water splitting using a nanosheet photocatalyst with single-atom reaction sites.