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Metal‐Free Fluorine‐Doped Carbon Electrocatalyst for CO2 Reduction Outcompeting Hydrogen Evolution
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-04-27 , DOI: 10.1002/anie.201802055 Jiafang Xie 1 , Xiaotao Zhao 1 , Maoxiang Wu 1 , Qiaohong Li 1 , Yaobing Wang 1 , Jiannian Yao 2
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-04-27 , DOI: 10.1002/anie.201802055 Jiafang Xie 1 , Xiaotao Zhao 1 , Maoxiang Wu 1 , Qiaohong Li 1 , Yaobing Wang 1 , Jiannian Yao 2
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The electrochemical CO2 reduction (ECDRR), as a key reaction in artificial photosynthesis to implement renewable energy conversion/storage, has been inhibited by the low efficiency and high costs of the electrocatalysts. Herein, we synthesize a fluorine‐doped carbon (FC) catalyst by pyrolyzing commercial BP 2000 with a fluorine source, enabling a highly selective CO2‐to‐CO conversion with a maximum Faradaic efficiency of 90 % at a low overpotential of 510 mV and a small Tafel slope of 81 mV dec−1, outcompeting current metal‐free catalysts. Moreover, the higher partial current density of CO and lower partial current density of H2 on FC relative to pristine carbon suggest an enhanced inherent activity towards ECDRR as well as a suppressed hydrogen evolution by fluorine doping. Fluorine doping activates the neighbor carbon atoms and facilitates the stabilization of the key intermediate COOH* on the fluorine‐doped carbon material, which are also blocked for competing hydrogen evolution, resulting in superior CO2‐to‐CO conversion.
中文翻译：
不含金属的氟掺杂碳电催化剂，可降低二氧化碳的排放，胜于氢的释放
作为人工光合作用中实现可再生能源转换/存储的关键反应，电化学CO 2还原（ECDRR）已被电催化剂的低效率和高成本所抑制。本文中，我们通过用氟源热解商用BP 2000合成了掺氟碳（FC）催化剂，实现了高选择性CO 2到CO的转化，在510 mV的低过电势下具有90％的最大法拉第效率。 Tafel斜率为81 mV dec -1的小斜率，胜过当前的无金属催化剂。而且，CO的部分电流密度较高，H 2的部分电流密度较低。相对于原始碳，FC上的碳原子分析表明对ECDRR的固有活性增强，并且氟掺杂抑制了氢的释放。氟掺杂会激活相邻的碳原子，并促进氟掺杂碳材料上关键中间体COOH *的稳定，而后者也因竞争氢的释放而被阻止，从而实现了出色的CO 2到CO转化。
更新日期：2018-04-27
中文翻译：
不含金属的氟掺杂碳电催化剂，可降低二氧化碳的排放，胜于氢的释放
作为人工光合作用中实现可再生能源转换/存储的关键反应，电化学CO 2还原（ECDRR）已被电催化剂的低效率和高成本所抑制。本文中，我们通过用氟源热解商用BP 2000合成了掺氟碳（FC）催化剂，实现了高选择性CO 2到CO的转化，在510 mV的低过电势下具有90％的最大法拉第效率。 Tafel斜率为81 mV dec -1的小斜率，胜过当前的无金属催化剂。而且，CO的部分电流密度较高，H 2的部分电流密度较低。相对于原始碳，FC上的碳原子分析表明对ECDRR的固有活性增强，并且氟掺杂抑制了氢的释放。氟掺杂会激活相邻的碳原子，并促进氟掺杂碳材料上关键中间体COOH *的稳定，而后者也因竞争氢的释放而被阻止，从而实现了出色的CO 2到CO转化。
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