共价有机框架纳米片中的高效电子传输用于高活性电催化二氧化碳还原
Efficient electron transmission in covalent organic framework nanosheets for highly active electrocatalytic carbon dioxide reduction.
作者信息
Zhu Hong-Jing, Lu Meng, Wang Yi-Rong, Yao Su-Juan, Zhang Mi, Kan Yu-He, Liu Jiang, Chen Yifa, Li Shun-Li, Lan Ya-Qian
机构信息
Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing, 210023, China.
Jiangsu Province Key Laboratory for Chemistry of Low-Dimensional Materials, School of Chemistry and Chemical Engineering, Huaiyin Normal University, Huai'an, 223300, China.
出版信息
Nat Commun. 2020 Jan 24;11(1):497. doi: 10.1038/s41467-019-14237-4.
Efficient conversion of carbon dioxide (CO) into value-added products is essential for clean energy research. Design of stable, selective, and powerful electrocatalysts for CO reduction reaction (CORR) 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 FE (91.3%, -0.7 V) and possess high cycling stability (>40 h). In addition, after exfoliation, the FE 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 FE can reach up to almost 100% (99.7%, -0.8 V). The electrocatalytic CORR mechanisms are discussed and revealed by density functional theory calculations. This work paves a new way in exploring porous crystalline materials in electrocatalytic CORR.
将二氧化碳（CO₂）高效转化为高附加值产品对于清洁能源研究至关重要。设计用于CO₂还原反应（CORR）的稳定、选择性和高效的电催化剂是非常有必要的，但在很大程度上尚未实现。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框架（M-TTCOFs）。四硫富瓦烯作为电子供体或载体，可以与金属卟啉构建定向电子传输途径。由此获得的M-TTCOFs可作为具有高法拉第效率（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）在-0.6至-0.9 V的宽电位范围内法拉第效率值高于90%，最大法拉第效率可达近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CORR机制。这项工作为探索多孔晶体材料在电催化CORR中的应用开辟了一条新途径。
Zotero 插件