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Boosting CO2 Electroreduction to CH4 via Tuning Neighboring Single-Copper Sites
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-02-06 , DOI: 10.1021/acsenergylett.0c00018
Anxiang Guan 1 , Zheng Chen 1 , Yueli Quan 1 , Chen Peng 1 , Zhiqiang Wang 2 , Tsun-Kong Sham 2 , Chao Yang 1 , Yali Ji 1 , Linping Qian 1 , Xin Xu 1 , Gengfeng Zheng 1
Affiliation  

We report single-atom Cu catalysts dispersed on nitrogen-doped carbon by a nitrogen-coordination strategy. The presence of nitrogen enabled good dispersion and attachment of atomic Cu species on the nitrogen-doped carbon frameworks with Cu–Nx configurations. The Cu doping concentrations and Cu–Nx configurations were well-tuned by the pyrolysis temperature. At a high Cu concentration of 4.9%mol, the distance between neighboring Cu–Nx species was close enough to enable C–C coupling and produce C2H4. In contrast, at Cu concentrations lower than 2.4%mol, the distance between Cu–Nx species was large so that the electrocatalyst favored the formation of CH4 as C1 products. Density functional theory calculations further confirmed the capability of producing C2H4 by two CO intermediates binding on two adjacent Cu–N2 sites, while the isolated Cu–N4, the neighboring Cu–N4, and the isolated Cu–N2 sites led to formation of CH4. Our work demonstrates a facile approach of tuning active Cu sites for CO2 electroreduction to different hydrocarbons.

中文翻译:

通过调整邻近的单铜位将CO 2电还原成CH 4

我们报告了通过氮配位策略分散在掺氮碳上的单原子铜催化剂。氮的存在使原子铜物种在具有Cu–N x构型的氮掺杂碳骨架上具有良好的分散性和附着性。铜的掺杂浓度和Cu–N x构型已通过热解温度进行了很好的调整。在4.9%mol的高Cu浓度下,相邻Cu–N x物种之间的距离足够近,可以进行C–C偶联并生成C 2 H 4。相反,当Cu浓度低于2.4%mol时,Cu–N x之间的距离物种很大,因此电催化剂有利于CH 4作为C 1产物的形成。密度泛函理论计算进一步证实了通过两个相邻的Cu–N 2位结合的CO中间体产生C 2 H 4的能力,而分离的Cu–N 4,相邻的Cu–N 4和分离的Cu–N 2位点导致形成CH 4。我们的工作证明了一种简便的方法,可以调节活性Cu位置以将CO 2电还原为不同的碳氢化合物。
更新日期:2020-02-06
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