Efficient Electrochemical Reduction of Carbon Dioxide to Acetate on Nitrogen-Doped Nanodiamond
Efficient Electrochemical Reduction of Carbon Dioxide to Acetate on Nitrogen-Doped Nanodiamond
复制标题
氮掺杂纳米金刚石上二氧化碳高效电化学还原为乙酸
DOI：
10.1021/jacs.5b02975
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发表时间：
2015-09-16
影响因子：
15
通讯作者：
Yu, Hongtao
中科院分区：
文献类型：
--
作者：
Liu, Yanming;Chen, Shuo;Yu, Hongtao
电化学还原CO2是一种有吸引力的减少CO2排放并将其转化为有用化学品的技术，但它存在过电位高、效率低或产物选择性差的问题。本文提出了n掺杂纳米金刚石/硅棒阵列（NDD/Si RA）作为一种高效的CO2还原非金属电催化剂。它优先且快速地将CO2转化为乙酸酯而不是甲酸酯，起始电位为-0.36 V (vs RHE)，克服了通常C2产物选择性低的限制。此外，在-0.8 ~ -1.0 V下，CO2还原效率达到了91.2 ~ 91.8%。其优异的CO2还原性能可归因于其高析氢过电位和N掺杂，其中N-sp(3)C对CO2还原具有高活性。电动力学数据和原位红外光谱显示CO2还原的主要途径可能是CO2 -> CO2中心点-> (COO)(2)（中心点）-> CH3COO-。
Electrochemical reduction of CO2 is an attractive technique for reducing CO2 emission and converting it into useful chemicals, but it suffers from high overpotential, low efficiency or poor product selectivity. Here, N-doped nanodiamond/Si rod array (NDD/Si RA) was proposed as an efficient nonmetallic electrocatalyst for CO2 reduction. It preferentially and rapidly converted CO2 to acetate over formate with an onset potential of -0.36 V (vs RHE), overcoming the usual limitation of low selectivity for C2 products. Moreover, faradic efficiency of 91.2-91.8% has been achieved for CO2 reduction at -0.8 to -1.0 V. Its superior performance for CO2 reduction can be attributed to its high overpotential for hydrogen evolution and N doping, where N-sp(3)C species was highly active for CO2 reduction. Electrokinetic data and in situ infrared spectrum revealed the main pathway for CO2 reduction might be CO2 -> CO2 center dot -> (COO)(2)(center dot)-> CH3COO-.