Bis(aminothiolato)nickel nanosheet as a redox switch for conductivity and an electrocatalyst for the hydrogen evolution reaction.
Bis(aminothiolato)nickel nanosheet as a redox switch for conductivity and an electrocatalyst for the hydrogen evolution reaction.
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DOI：
10.1039/c7sc02688a
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发表时间：
2017-12-01
期刊：
影响因子：
8.4
通讯作者：
Nishihara H
中科院分区：
文献类型：
--
作者：
Sun X;Wu KH;Sakamoto R;Kusamoto T;Maeda H;Ni X;Jiang W;Liu F;Sasaki S;Masunaga H;Nishihara H
精确调控的功能性配位纳米片对HER表现出很好的催化活性，并伴随着氧化还原处理引起的电子性质的急剧转变。通过Ni（acac）2与1，3，5-三氨基苯-2，4，6-三硫醇在液-液和气-液界面上的反应，合成了一种含有双（氨基硫醇基）镍（NiAT）的π共轭配位纳米片.片材厚度可以控制到单层（0.6nm）。选区电子衍射和掠入射X-射线衍射分析表明，形成了一个平坦的结晶片与kagome晶格堆叠在交错排列。NiAT通过2 H +-2e-化学反应可逆地相互转化为双（亚氨基硫醇基）镍（NiIT）纳米片，伴随着电导率从3 × 10-6到1 × 10-1 S cm-1的急剧变化。这种电导率的变化是由NiAT和NiIT之间的能带结构的差异来解释的。NiAT作为一种有效的析氢电催化剂，表现出很强的耐酸性和-0.15 V的起始过电位。
Precisely tuned functional coordination nanosheet exhibits competent catalytic activity for HER, accompany with drastic electronic property switching by redox treatment. A π-conjugated coordination nanosheet comprising bis(aminothiolato)nickel (NiAT) moieties was synthesized by the reaction of Ni(acac)2 with 1,3,5-triaminobenzene-2,4,6-trithiol at liquid–liquid and gas–liquid interfaces. The sheet thickness could be controlled down to a single layer (0.6 nm). Selected area electron diffraction and grazing incidence X-ray diffraction analyses indicated the formation of a flat crystalline sheet with a kagome lattice stacked in a staggered alignment. NiAT was reversibly interconverted to a bis(iminothiolato)nickel (NiIT) nanosheet by the chemical 2H+–2e– reaction, which was accompanied by a drastic change in electrical conductivity from 3 × 10–6 to 1 × 10–1 S cm–1. This change in conductivity was explained by the difference in band structures between NiAT and NiIT. NiAT acted as an efficient electrocatalyst for the hydrogen evolution reaction, showing strong acid durability and an onset overpotential of –0.15 V.
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