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Efficient Conversion of Carbon Dioxide on Atomically Dispersed Metal–Nx Species-Anchored Porous Carbon with Embedded CuxCoy Nanoparticles by Accelerating Electron Separation
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-03-30 , DOI: 10.1021/acssuschemeng.0c00652 Jun Cheng 1 , Xiao Yang 1 , Xiaoxu Xuan 1 , Niu Liu 1 , Junhu Zhou 1
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-03-30 , DOI: 10.1021/acssuschemeng.0c00652 Jun Cheng 1 , Xiao Yang 1 , Xiaoxu Xuan 1 , Niu Liu 1 , Junhu Zhou 1
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To promote methanol product selectivity in CO2 reduction through photoelectrochemical reactions, a novel hybrid electrocatalyst (CuCo/NC) was developed to enhance electron transfer from cobalt to copper atoms with coordinated nitrogen on a ZIF-derived carbon matrix. The binding energies of Co 2p3/2 in CuCo/NC exhibited a 0.2 eV shifting to lower values, whereas those of Cu 2p3/2 exhibited a lower value shift by 1.5 eV, both of which contributed to electron transfer from Co to Cu. DFT calculations showed that the C–Co bond length (1.808 Å) between the CO* intermediate and CuCo/NC electrocatalyst was shorter than those in Cu/NC and Co/NC (1.946 and 1.870 Å, respectively), indicating that CO* was easier to adsorb on the CuCo/NC electrocatalyst for further reduction. The CuCo/NC electrocatalyst with stable properties efficiently converted CO2 into methanol (FE > 60%) with a carbon atom conversion rate of 4098 nmol h–1 cm–2.
中文翻译：
通过加速电子分离，在具有嵌入式CuxCoy纳米粒子的原子分散的金属-Nx物种锚固多孔碳上有效转化二氧化碳
促进甲醇产品在CO 2中的选择性通过光电化学反应的还原，开发了一种新型的混合电催化剂（CuCo / NC），以增强电子在ZIF衍生的碳基质上与钴之间的配位氮从钴到铜原子的转移。在CuCo / NC中，Co 2p3 / 2的键合能表现出0.2 eV的偏移，直至更低的值，而Cu 2p3 / 2的键合能表现出的较低的值偏移1.5 eV，这两者都有助于电子从Co转移到Cu。DFT计算表明，CO *中间体与CuCo / NC电催化剂之间的C–Co键长（1.808Å）短于Cu / NC和Co / NC的C–Co键长（分别为1.946和1.870Å），表明CO *为更易于吸附在CuCo / NC电催化剂上以进一步还原。具有稳定性能的CuCo / NC电催化剂可有效转化CO 2转化为甲醇（FE> 60％），碳原子转化率为4098 nmol h –1 cm –2。
更新日期：2020-04-23
中文翻译：
通过加速电子分离，在具有嵌入式CuxCoy纳米粒子的原子分散的金属-Nx物种锚固多孔碳上有效转化二氧化碳
促进甲醇产品在CO 2中的选择性通过光电化学反应的还原，开发了一种新型的混合电催化剂（CuCo / NC），以增强电子在ZIF衍生的碳基质上与钴之间的配位氮从钴到铜原子的转移。在CuCo / NC中，Co 2p3 / 2的键合能表现出0.2 eV的偏移，直至更低的值，而Cu 2p3 / 2的键合能表现出的较低的值偏移1.5 eV，这两者都有助于电子从Co转移到Cu。DFT计算表明，CO *中间体与CuCo / NC电催化剂之间的C–Co键长（1.808Å）短于Cu / NC和Co / NC的C–Co键长（分别为1.946和1.870Å），表明CO *为更易于吸附在CuCo / NC电催化剂上以进一步还原。具有稳定性能的CuCo / NC电催化剂可有效转化CO 2转化为甲醇（FE> 60％），碳原子转化率为4098 nmol h –1 cm –2。
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