Study of the Active Sites in Porous Nickel Oxide Nanosheets by Manganese Modulation for Enhanced Oxygen Evolution Catalysis

Study of the Active Sites in Porous Nickel Oxide Nanosheets by Manganese Modulation for Enhanced Oxygen Evolution Catalysis
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通过锰调节增强析氧催化的多孔氧化镍纳米片活性位点的研究

DOI:
10.1021/acsenergylett.8b01206
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发表时间:
2018-08
期刊:
影响因子:
22
通讯作者:
Ding Yong
Ding Yong
中科院分区:
材料科学1区
文献类型:
--
作者:
Tian Tian;Gao Hong;Zhou Xichen;Zheng Lirong;Wu Jianfeng;Li Kai;Ding Yong

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确定析氧反应催化剂的活性中心是研究水氧化反应机理的基础。在电催化析氧体系中,研究了锰调制氧化镍纳米片的活性中心。电子结构可以通过Mn调制来实现。Ni3+(T2g6eg1)和Jahn-Teller活性Mn3+(T2g3eg1)物种的本征催化活性协同促进了电催化析氧反应。X射线吸收近边结构分析表明,Ni0.75Mn0.25纳米板材中的Ni3+和Mn3+分别来自于镍空位和氧空位。所得Ni0.75Mn0.25纳米薄片的析氧活性远高于NiO和Mn2O。密度泛函理论计算表明,Ni和Mn协同作用促进O-O键的形成。我们的工作提供了对多孔氧化镍纳米片的活性中心的全面理解。
Identifying active sites of oxygen evolution reaction catalysts is essential for studying water oxidation mechanisms. Herein, the active site of nickel oxide nanosheets by manganese modulation is investigated in an electrocatalytic oxygen evolution system. The electronic structure could be realized by Mn modulation. The intrinsic catalytic activity of Ni3+ (t2g6eg1) and Jahn–Teller active Mn3+ (t2g3eg1) species act synergistically to promote the elctrocatalytic oxygen evolution reaction. X-ray absorption near-edge structure analysis indicates that the Ni3+ and Mn3+ in Ni0.75Mn0.25 nanosheets should result from nickel vacancies and oxygen vacancies, respectively. The resulting Ni0.75Mn0.25 nanosheets show much higher oxygen evolution activity than those of NiO and Mn2O3. Density functional theory calculations indicate that the Ni and Mn act synergistically to promote formation of the O–O bond. Our work provides a comprehensive understanding of the active site of porous nickel oxide nanosheets by manganese ...