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Efficient electron transmission in covalent organic framework nanosheets for highly active electrocatalytic carbon dioxide reduction.
Nature Communications ( IF 14.7 ) Pub Date : 2020-01-24 , DOI: 10.1038/s41467-019-14237-4
Hong-Jing Zhu 1 , Meng Lu 1 , Yi-Rong Wang 1 , Su-Juan Yao 1 , Mi Zhang 1 , Yu-He Kan 2 , Jiang Liu 1 , Yifa Chen 1 , Shun-Li Li 1 , Ya-Qian Lan 1
Affiliation  

Efficient conversion of carbon dioxide (CO2) into value-added products is essential for clean energy research. Design of stable, selective, and powerful electrocatalysts for CO2 reduction reaction (CO2RR) is highly desirable yet largely unmet. In this work, a series of metalloporphyrin-tetrathiafulvalene based covalent organic frameworks (M-TTCOFs) are designed. Tetrathiafulvalene, serving as electron donator or carrier, can construct an oriented electron transmission pathway with metalloporphyrin. Thus-obtained M-TTCOFs can serve as electrocatalysts with high FECO (91.3%, -0.7 V) and possess high cycling stability (>40 h). In addition, after exfoliation, the FECO value of Co-TTCOF nanosheets (~5 nm) is higher than 90% in a wide potential range from -0.6 to -0.9 V and the maximum FECO can reach up to almost 100% (99.7%, -0.8 V). The electrocatalytic CO2RR mechanisms are discussed and revealed by density functional theory calculations. This work paves a new way in exploring porous crystalline materials in electrocatalytic CO2RR.

中文翻译:

共价有机骨架纳米片中的高效电子传输,可实现高活性的电催化二氧化碳还原。

将二氧化碳(CO2)有效转化为增值产品对于清洁能源研究至关重要。设计用于CO2还原反应(CO2RR)的稳定,选择性和功能强大的电催化剂是非常需要的,但很大程度上尚未得到满足。在这项工作中,设计了一系列基于金属卟啉-四硫富瓦烯的共价有机骨架(M-TTCOF)。四硫富瓦烯用作电子供体或载体,可以与金属卟啉构成定向的电子传输途径。如此获得的M-TTCOF可以用作具有高FECO(91.3%,-0.7 V)的电催化剂,并具有高循环稳定性(> 40 h)。此外,剥离后,Co-TTCOF纳米片(〜5 nm)的FECO值在-0.6至-0.9 V的宽电位范围内均高于90%,最大FECO可以达到近100%(99.7%) ,-0.8 V)。通过密度泛函理论计算讨论并揭示了电催化CO2RR机理。这项工作为探索电催化CO2RR中的多孔晶体材料开辟了一条新途径。
更新日期:2020-01-24
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