Highly Selective Photoreduction of CO2 with Suppressing H-2 Evolution by Plasmonic Au/CdSe-Cu2O Hierarchical Nanostructures under Visible Light
Highly Selective Photoreduction of CO2 with Suppressing H-2 Evolution by Plasmonic Au/CdSe-Cu2O Hierarchical Nanostructures under Visible Light
复制标题
可见光下等离子体 Au/CdSe·Cu2O 多级纳米结构高选择性光还原 CO2 并抑制 H2 析出
DOI：
10.1002/smll.202000426
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发表时间：
2020
期刊：
影响因子：
13.3
通讯作者：
Zhang Jiatao
中科院分区：
文献类型：
--
作者：
Wang Hongzhi;Rong Hongpan;Wang Dong;Li Xinyuan;Zhang Erhuan;Wan Xiaodong;Bai Bing;Xu Meng;Liu Jiajia;Liu Jia;Chen Wenxing;Zhang Jiatao
在可见光（λ > 420 nm）照射下，通过完全抑制析氢反应，实现了碳产物选择性高达100%的光催化CO2还原反应（CO2 RR）。为了实现这一目标，等离子体Au/CdSe哑铃状纳米棒增强了光捕获，并产生了等离子体增强的富电荷环境;外围Cu 2 O为CO2还原提供了丰富的活性位点，并抑制了氢的生成，以提高碳产物的选择性。中间的CdSe充当桥来转移光电荷。基于这些Au/CdSe-Cu 2 O分级纳米结构（HNS）的合成，可以实现有效的光致电子/空穴（e-/h+）分离和100%的CO选择性。此外，CO的2 e −/2 H+产物可以进一步增强和氢化，以有效地完成CO2到甲烷（CH 4）的8 e −/8H+还原，其中足够的CO浓度和H2O还原提供的质子是必不可少的。在最佳条件下，Au/CdSe-Cu 2 O HNS具有较高的光催化活性和稳定性，在60 h内，CO和CH 4的稳定产气速率分别为254和123 μmol g−1h− 1.
Here, the photocatalytic CO2reduction reaction (CO2RR) with the selectivity of carbon products up to 100% is realized by completely suppressing the H2evolution reaction under visible light (λ > 420 nm) irradiation. To target this, plasmonic Au/CdSe dumbbell nanorods enhance light harvesting and produce a plasmon‐enhanced charge‐rich environment; peripheral Cu2O provides rich active sites for CO2reduction and suppresses the hydrogen generation to improve the selectivity of carbon products. The middle CdSe serves as a bridge to transfer the photocharges. Based on synthesizing these Au/CdSe–Cu2O hierarchical nanostructures (HNSs), efficient photoinduced electron/hole (e−/h+) separation and 100% of CO selectivity can be realized. Also, the 2e−/2H+products of CO can be further enhanced and hydrogenated to effectively complete 8e−/8H+reduction of CO2to methane (CH4), where a sufficient CO concentration and the proton provided by H2O reduction are indispensable. Under the optimum condition, the Au/CdSe–Cu2O HNSs display high photocatalytic activity and stability, where the stable gas generation rates are 254 and 123 µmol g−1h−1for CO and CH4over a 60 h period.