Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction,ACS Central Science

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Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction
ACS Central Science ( IF 12.7 ) Pub Date : 2017-09-13 00:00:00 , DOI: 10.1021/acscentsci.7b00316
Ming Gong , Zhi Cao , Wei Liu , Eva M. Nichols , Peter T. Smith , Jeffrey S. Derrick , Yi-Sheng Liu , Jinjia Liu ₁ , Xiaodong Wen _{1,

2} , Christopher J. Chang

Affiliation

Conversion of carbon monoxide (CO), a major one-carbon product of carbon dioxide (CO₂) reduction, into value-added multicarbon species is a challenge to addressing global energy demands and climate change. Here we report a modular synthetic approach for aqueous electrochemical CO reduction to carbon–carbon coupled products via self-assembly of supramolecular cages at molecular–materials interfaces. Heterobimetallic cavities formed by face-to-face coordination of thiol-terminated metalloporphyrins to copper electrodes through varying organic struts convert CO to C2 products with high faradaic efficiency (FE = 83% total with 57% to ethanol) and current density (1.34 mA/cm²) at a potential of −0.40 V vs RHE. The cage-functionalized electrodes offer an order of magnitude improvement in both selectivity and activity for electrocatalytic carbon fixation compared to parent copper surfaces or copper functionalized with porphyrins in an edge-on orientation.

中文翻译：

超分子卟啉笼组装在分子材料界面上用于电催化还原CO

一氧化碳（CO）是二氧化碳（CO ₂）还原的主要一种碳产物，将其转化为增值的多碳物种是解决全球能源需求和气候变化的挑战。在这里，我们报告了一种模块化合成方法，该方法通过在分子材料界面处自组装超分子笼，将水性电化学CO还原为碳-碳偶联产物。硫醇封端的金属卟啉通过不同的有机支撑物与铜电极的面对面配位形成的异双金属腔体将CO转化为具有高法拉第效率（FE = 83％总计57％转化为乙醇）的C2产品和电流密度（1.34 mA /厘米²）在相对于RHE为-0.40 V的电势下。与母体铜表面或在边缘取向上用卟啉功能化的铜相比，笼式官能化的电极在电催化碳固定方面的选择性和活性均提高了一个数量级。

更新日期：2017-09-13

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