Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-03-19 , DOI: 10.1016/j.apcatb.2020.118908 Shaohua Feng , Wanzhen Zheng , Jingke Zhu , Zhongjian Li , Bin Yang , Zhenhai Wen , Jianguo Lu , Lecheng Lei , Shaobin Wang , Yang Hou
Electrochemical reduction of CO2 (ECR-CO2) into high value-added products plays a crucial role in energy conversions. Herein, we developed a family of porous metal-porphyrin triazine-based frameworks (MPTFs-x, M = Mn, Fe, Co, Ni, and Cu, x = temperature) with a specific surface area up to 977 m2 g-1 and homogenously dispersed transition-metals. Benefiting from a high content of N species of 8.43 at.% and abundantly exposed Ni-Nx active sites, NiPTFs-600 displayed a superb Faradaic efficiency (FE) of CO production (> 90%) in the range of -0.55 V to -0.95 V with the maximum FE of 97.6% and current density of 10.8 mA cm-2 at -0.8 V. The reaction mechanism was found to be the adsorption of CO2 molecules to form *CO2 intermediates, accompanied by successive protonation to produce *COOH and then *CO.
中文翻译:
基于多孔金属卟啉三嗪的骨架,可有效还原CO 2
将CO 2(ECR-CO 2)电化学还原为高附加值产品在能量转换中起着至关重要的作用。在此,我们开发了比表面积最大为977 m 2 g -1的多孔金属-卟啉三嗪基骨架(MPTFs-x,M = Mn,Fe,Co,Ni和Cu,x =温度)。和均匀分散的过渡金属。NiPTFs-600得益于高含量的8.43 at。%的N物种和大量暴露的Ni-N x活性位,在-0.55 V至0.55 V的范围内显示出了极好的法拉第效率(FE),CO产生率(> 90%)。 -0.95 V,最大FE为97.6%,电流密度为10.8 mA cm -2在-0.8V下发现反应机理。该机理是吸附CO 2分子以形成* CO 2中间体,并伴随着连续质子化以生成* COOH,然后生成* CO。