Atomically dispersed nickel-nitrogen-sulfur species anchored on porous carbon nanosheets for efficient water oxidation
Atomically dispersed nickel-nitrogen-sulfur species anchored on porous carbon nanosheets for efficient water oxidation
复制标题
原子分散的镍-氮-硫物质锚定在多孔碳纳米片上，可有效氧化水
DOI：
10.1038/s41467-019-09394-5
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发表时间：
2019-03-27
影响因子：
16.6
通讯作者：
Feng, Xinliang
中科院分区：
文献类型：
--
作者：
Hou, Yang;Qiu, Ming;Feng, Xinliang
开发低成本的电催化剂以取代昂贵的铱基材料是析氧反应（OER）的关键。在这里，我们报告了原子分散的镍与多孔碳纳米片中的氮和硫物种配位，作为一种电催化剂，表现出优异的OER活性和耐久性，在10 mA cm（-2）下具有1.51 V的低过电位，并且在碱性介质中具有45 mV dec（-1）的小塔菲尔斜率。这种电催化剂代表了所有报道的过渡金属和/或杂原子掺杂的碳电催化剂中最好的，并且甚至上级于基准Ir/C。理论和实验结果表明，分子中分散良好的S垂直棒状NiNx物种是催化OER的活性中心。通过像差校正的扫描透射电子显微镜和同步辐射X射线吸收光谱以及计算机模拟，清楚地揭示了碳基质中S垂直棒NiNx中心的原子结构。Fe 2 O3纳米片阵列上的纳米碳集成光电阳极能够实现高度活性的太阳能驱动的氧气生产。
Developing low-cost electrocatalysts to replace precious Ir-based materials is key for oxygen evolution reaction (OER). Here, we report atomically dispersed nickel coordinated with nitrogen and sulfur species in porous carbon nanosheets as an electrocatalyst exhibiting excellent activity and durability for OER with a low overpotential of 1.51 V at 10 mA cm(-2) and a small Tafel slope of 45 mV dec(-1) in alkaline media. Such electrocatalyst represents the best among all reported transition metal- and/or heteroatom-doped carbon electrocatalysts and is even superior to benchmark Ir/C. Theoretical and experimental results demonstrate that the well-dispersed molecular S vertical bar NiNx species act as active sites for catalyzing OER. The atomic structure of S vertical bar NiNx centers in the carbon matrix is clearly disclosed by aberration-corrected scanning transmission electron microscopy and synchrotron radiation X-ray absorption spectroscopy together with computational simulations. An integrated photoanode of nanocarbon on a Fe2O3 nanosheet array enables highly active solar-driven oxygen production.