Temperature Effect of CO2 Reduction Electrocatalysis on Copper: Potential Dependency of Activation Energy
Temperature Effect of CO2 Reduction Electrocatalysis on Copper: Potential Dependency of Activation Energy
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CO2 还原电催化对铜的温度影响：活化能的潜在依赖性
DOI：
10.1115/1.4046552
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发表时间：
2020
影响因子：
2.5
通讯作者：
Suntivich, Jin
中科院分区：
文献类型：
--
作者：
Zong, Yixu;Chakthranont, Pongkarn;Suntivich, Jin
在过去的十年中，电化学二氧化碳还原反应(CO2RR)作为能源和燃料可持续发展的一个组成部分，受到了广泛的关注。铜是为数不多的能将二氧化碳转化为高阶烃的电催化剂之一。我们报道了从5°C到45°C的多晶铜的CO_2RR随电化学势的变化。结果表明，与可逆氢电极相比，在−0.95V~−1.25V的电位值范围内，甲烷在低温下的选择性向甲烷转移，在高温下向H_2的选择性转移。我们分析了每个产物的活化能，并基于它们的潜在依赖性讨论了可能的潜在机制。CH4的活化势垒符合Butler-Volmer方程，而C2H4和CO则表现出不平凡的趋势。我们的结果表明，CH4的产生是通过经典的电化学途径进行的，很可能是表面饱和的CoAD的质子耦合电子转移，而C2H4受到更复杂的过程的限制，可能涉及表面吸附。我们的测量结果与吸附-吸附相互作用决定C2+选择性的观点是一致的。
The electrochemical CO2reduction reaction (CO2RR) has gathered widespread attention in the past decade as an enabling component to energy and fuel sustainability. Copper (Cu) is one of the few electrocatalysts that can convert CO2to higher-order hydrocarbons. We report the CO2RR on polycrystalline Cu from 5 °C to 45 °C as a function of electrochemical potential. Our result shows that selectivity shifts toward CH4at low temperature and H2at high temperature at the potential values between −0.95 V and −1.25 V versus reversible hydrogen electrode (RHE). We analyze the activation energy for each product and discuss the possible underlying mechanism based on their potential dependence. The activation barrier of CH4empirically obeys the Butler–Volmer equation, while C2H4and CO show a non-trivial trend. Our result suggests that the CH4production proceeds via a classical electrochemical pathway, likely the proton-coupled electron transfer of surface-saturated COad, while C2H4is limited by a more complex process, likely involving surface adsorbates. Our measurement is consistent with the view that the adsorbate–adsorbate interaction dictates the C2+selectivity.
影响因子：
3.9
作者：
Engelbrecht, Andreas;Uhlig, Conrad;Moos, Ralf
通讯作者：
Moos, Ralf
用于二氧化碳电解还原的气体扩散层上脉冲镀铜
DOI：
--
发表时间：
2018
期刊：
影响因子：
--
作者：
S. Sen;McLain E. Leonard;R. Radhakrishnan;S. Snyder;B. Skinn;Dan Wang;Timothy D. Hall;E. Taylor;F. Brushett
通讯作者：
F. Brushett