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Electrochemical reduction of CO2 to synthesis gas with controlled CO/H2 ratios
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2017-02-20 00:00:00 , DOI: 10.1039/c7ee00071e Wenchao Sheng 1, 2, 3, 4 , Shyam Kattel 4, 5, 6, 7 , Siyu Yao 4, 5, 6, 7 , Binhang Yan 4, 5, 6, 7 , Zhixiu Liang 4, 5, 6, 7 , Christopher J. Hawxhurst 1, 2, 3, 4 , Qiyuan Wu 4, 8, 9, 10 , Jingguang G. Chen 1, 2, 3, 4, 5
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2017-02-20 00:00:00 , DOI: 10.1039/c7ee00071e Wenchao Sheng 1, 2, 3, 4 , Shyam Kattel 4, 5, 6, 7 , Siyu Yao 4, 5, 6, 7 , Binhang Yan 4, 5, 6, 7 , Zhixiu Liang 4, 5, 6, 7 , Christopher J. Hawxhurst 1, 2, 3, 4 , Qiyuan Wu 4, 8, 9, 10 , Jingguang G. Chen 1, 2, 3, 4, 5
Affiliation
The electrochemical carbon dioxide reduction reaction (CO2RR) to simultaneously produce carbon monoxide (CO) and hydrogen (H2) has been achieved on carbon supported palladium (Pd/C) nanoparticles in an aqueous electrolyte. The synthesis gas product has a CO to H2 ratio between 0.5 and 1, which is in the desirable range for thermochemical synthesis of methanol and Fischer–Tropsch reactions using existing industrial processes. In situ X-ray absorption spectroscopy in both near-edge (XANES) and extended regions (EXAFS) and in situ X-ray diffraction show that Pd has transformed into β-phase palladium hydride (β-PdH) during the CO2RR. Density functional theory (DFT) calculations demonstrate that the binding energies of both adsorbed CO and H are significantly weakened on PdH than on Pd surfaces, and that these energies are potential descriptors to facilitate the search for more efficient electrocatalysts for syngas production through the CO2RR.
中文翻译:
以受控的CO / H 2比率将CO 2电化学还原为合成气
已经在水性电解质中的碳载钯(Pd / C)纳米粒子上实现了同时产生一氧化碳(CO)和氢(H 2)的电化学二氧化碳还原反应(CO 2 RR)。合成气产品的CO与H 2之比在0.5和1之间,这在使用现有工业工艺进行甲醇和费托反应的热化学合成中处于理想的范围。近边缘(XANES)和扩展区域(EXAFS)的原位X射线吸收光谱法和原位X射线衍射表明,CO 2期间Pd已转变为β相氢化钯(β-PdH)。RR。密度泛函理论(DFT)计算表明,吸附的CO和H的结合能在PdH上比在Pd表面上显着减弱,并且这些能量是潜在的描述符,有助于寻找更有效的电催化剂,以通过CO 2产生合成气RR。
更新日期:2017-05-31
中文翻译:
以受控的CO / H 2比率将CO 2电化学还原为合成气
已经在水性电解质中的碳载钯(Pd / C)纳米粒子上实现了同时产生一氧化碳(CO)和氢(H 2)的电化学二氧化碳还原反应(CO 2 RR)。合成气产品的CO与H 2之比在0.5和1之间,这在使用现有工业工艺进行甲醇和费托反应的热化学合成中处于理想的范围。近边缘(XANES)和扩展区域(EXAFS)的原位X射线吸收光谱法和原位X射线衍射表明,CO 2期间Pd已转变为β相氢化钯(β-PdH)。RR。密度泛函理论(DFT)计算表明,吸附的CO和H的结合能在PdH上比在Pd表面上显着减弱,并且这些能量是潜在的描述符,有助于寻找更有效的电催化剂,以通过CO 2产生合成气RR。