A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction
A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction
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DOI：
10.1021/jacs.6b02878
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发表时间：
2016-07-06
影响因子：
15
通讯作者：
Chang, Christopher J.
中科院分区：
文献类型：
--
作者：
Cao, Zhi;Kim, Dohyung;Chang, Christopher J.
将温室气体二氧化碳（CO2）转化为增值产品是可持续能源研究的一个重要挑战，而纳米材料为这种转化提供了广泛的多相催化剂。本文报道了一种分子表面功能化方法来调整金纳米粒子（Au NP）电催化剂，使其将CO2还原为CO。n -杂环（NHC）碳功能化的Au NP催化剂在中性pH下，过电位为0.46 V时，在水中将CO2还原为CO的法拉第效率（FE = 83%）提高，电流密度比母体Au NP （FE = 53%）提高了7.6倍。NHC碳功能化Au NP （72 mV/ 10年）与亲本Au NP （138 mV/ 10年）体系的Tafel图进一步表明，分子配体影响了CO2还原的机制途径。结果建立了分子表面功能化作为纳米颗粒催化剂设计的尺寸，形状，组成和缺陷控制的补充方法。
Conversion of the greenhouse gas carbon dioxide (CO2) to value-added products is an important challenge for sustainable energy research, and nanomaterials offer a broad class of heterogeneous catalysts for such transformations. Here we report a molecular surface functionalization approach to tuning gold nanoparticle (Au NP) electrocatalysts for reduction of CO2 to CO. The N-heterocyclic (NHC) carbene-functionalized Au NP catalyst exhibits improved faradaic efficiency (FE = 83%) for reduction of CO2 to CO in water at neutral pH at an overpotential of 0.46 V with a 7.6-fold increase in current density compared to that of the parent Au NP (FE = 53%). Tafel plots of the NHC carbene-functionalized Au NP (72 mV/decade) vs parent Au NP (138 mV/decade) systems further show that the molecular ligand influences mechanistic pathways for CO2 reduction. The results establish molecular surface functionalization as a complementary approach to size, shape, composition, and defect control for nanoparticle catalyst design.