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Promoting C2+ Production from Electrochemical CO2 Reduction on Shape-Controlled Cuprous Oxide Nanocrystals with High-Index Facets
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-09-16 , DOI: 10.1021/acssuschemeng.0c04873
Wenli Fu 1 , Zhen Liu 2 , Tanyuan Wang 1 , Jiashun Liang 1 , Shuo Duan 1 , Linfeng Xie 1 , Jiantao Han 1 , Qing Li 1
Affiliation  

Morphology- and crystal facet-controlled Cu2O nanocrystals (NCs), including cubic Cu2O (c-Cu2O) NCs with {100} facets, rhombic dodecahedral Cu2O (d-Cu2O) NCs with {110} facets, and concave octahedral Cu2O (o-Cu2O) NCs with high-index facets, are prepared and employed as catalysts for the electrochemical reduction of CO2 to C2+ products (ethylene, ethanol, and n-propanol). In situ Raman characterizations demonstrate that the surfaces of all three Cu2O NCs are rapidly converted to metallic Cu during CO2 reduction and reoxidized to smaller-sized Cu2O NCs after tests. Specifically, the o-Cu2O catalyst reveals the highest Faradaic efficiency (48.3%) and partial current density (17.7 mA cm–2) for C2+ products at −1.1 V versus reversible hydrogen electrode compared to c-Cu2O and d-Cu2O, which is competitive among the reported Cu and Cu2O catalysts. In addition, abundant crystal defects/grain boundaries and high-index facets are observed on the surface of reconstructed o-Cu2O, which may serve as the active sites and benefit the C–C coupling during CO2 reduction. This work provides a new strategy to achieve efficient C2+ production from electrochemical CO2 reduction via crystal facet regulation of Cu2O catalysts.

中文翻译:

促进形状控制的高折射率小平面氧化亚铜纳米晶体上电化学还原CO 2产生的C 2+。

形态和晶面控制的Cu 2 O纳米晶体(NCs),包括具有{100}面的立方Cu 2 O(c-Cu 2 O)NCs,具有{110的菱形十二面体Cu 2 O(d-Cu 2 O)NCs }刻面,和凹八面体的Cu 2 O(邻-铜2 O)与高指数晶面NCS,制备并用作催化剂的电化学还原的CO 2到C 2+产品(乙烯,乙醇和ñ丙醇)。原位拉曼光谱表征表明,所有三个Cu 2 O NC的表面在CO 2期间均迅速转化为金属Cu在测试后还原并再氧化为较小尺寸的Cu 2 O NCs。具体而言,邻的Cu 2 O类催化剂揭示了最高法拉第效率(48.3%)和部分的电流密度(17.7毫安厘米-2)对于C 2+产品在-1.1 V相对于可逆氢电极相比C-的Cu 2 O和d-Cu 2 O,在所报道的Cu和Cu 2 O催化剂中具有竞争力。此外,在重构的o-Cu 2 O表面观察到大量的晶体缺陷/晶界和高折射率小平面,这可能是活性位点,并有利于CO 2期间的C–C耦合。减少。这项工作提供了一种新的策略,可通过对Cu 2 O催化剂进行晶面调节,从电化学CO 2还原中获得高效的C 2+生产。
更新日期:2020-10-12
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