Chinese Journal of Catalysis ( IF 16.5 ) Pub Date : 2022-05-21 , DOI: 10.1016/s1872-2067(21)64006-8 Chuhao Liu, Yue Wu, Jinjie Fang, Ke Yu, Hui Li, Wenjun He, Weng-Chon Cheong, Shoujie Liu, Zheng Chen, Jing Dong, Chen Chen
The use of carbon-based materials is an appealing strategy to solve the issue of excessive CO2 emissions. In particular, metal-free nitrogen-doped carbon materials (mf-NCs) have the advantages of convenient synthesis, cost-effectiveness, and high conductivity and are ideal electrocatalysts for the CO2 reduction reaction (CO2RR). However, the unclear identification of the active N sites and the low intrinsic activity of mf-NCs hinder the further development of high-performance CO2RR electrocatalysts. Achieving precise control over the synthesis of mf-NC catalysts with well-defined active N-species sites is still challenging. To this end, we adopted a facile synthesis method to construct a set of mf-NCs as robust catalysts for CO2RR. The resulting best-performing catalyst obtained a Faradaic efficiency of CO of approximately 90% at −0.55 V (vs. reversible hydrogen electrode) and good stability. The electrocatalytic performance and in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy measurements collectively revealed that graphitic and pyridinic N can synergistically adsorb CO2 and H2O and thus promote CO2 activation and protonation.
中文翻译:
氮掺杂碳催化剂对高效电化学 CO2 还原的协同作用
使用碳基材料是解决过量 CO 2排放问题的一种有吸引力的策略。特别是无金属氮掺杂碳材料(mf-NCs)具有合成方便、成本效益高、电导率高等优点,是理想的CO 2还原反应(CO 2 RR)电催化剂。然而,活性N位点的识别不明确和mf-NCs的低固有活性阻碍了高性能CO 2 RR电催化剂的进一步发展。实现对具有明确定义的活性 N 物种位点的 mf-NC 催化剂的合成的精确控制仍然具有挑战性。为此,我们采用一种简便的合成方法构建了一组 mf-NCs 作为 CO 的稳健催化剂2 RR。由此产生的性能最佳的催化剂在 -0.55 V(相对于可逆氢电极)下获得了约 90% 的 CO 法拉第效率和良好的稳定性。电催化性能和原位衰减全反射表面增强红外吸收光谱测量共同表明石墨和吡啶N可以协同吸附CO 2和H 2 O,从而促进CO 2活化和质子化。