A bio-inspired O 2 -tolerant catalytic CO 2 reduction electrode

Lu，Xu1,2; Jiang，Zhan3; Yuan，Xiaolei1,2,4; Wu，Yueshen1,2; Malpass-Evans，Richard5; Zhong，Yiren1,2; Liang，Yongye3; McKeown，Neil B.5; Wang，Hailiang1,2

2019

10.1016/j.scib.2019.04.008

Science Bulletin   影响因子和分区

2095-9273

2095-9281

The electrochemical reduction of CO to give CO in the presence of O would allow the direct valorization of flue gases from fossil fuel combustion and of CO captured from air. However, it is a challenging task because O reduction is thermodynamically favored over that of CO . 5% O in CO near catalyst surface is sufficient to completely inhibit the CO reduction reaction. Here we report an O -tolerant catalytic CO reduction electrode inspired by part of the natural photosynthesis unit. The electrode comprises of heterogenized cobalt phthalocyanine molecules serving as the cathode catalyst with >95% Faradaic efficiency (FE) for CO reduction to CO coated with a polymer of intrinsic microporosity that works as a CO -selective layer with a CO /O selectivity of ∼20. Integrated into a flow electrolytic cell, the hybrid electrode operating with a CO feed gas containing 5% O exhibits a FE of 75.9% with a total current density of 27.3 mA/cm at a cell voltage of 3.1 V. A FE of 49.7% can be retained when the O fraction increases to 20%. Stable operation for 18 h is demonstrated. The electrochemical performance and O tolerance can be further enhanced by introducing cyano and nitro substituents to the phthalocyanine ligand.

Cooperative catalysis Electrochemical CO 2 reduction Gas separation O 2 tolerance Polymer of intrinsic microporosity

EI ; SCI

英语

通讯

Institute of International Education[] ; Shenzhen Fundamental Research and Discipline Layout project[JCYJ20160608140827794] ; [CHE-1651717]

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:000502833900008

Elsevier B.V.

20191606776858

Catalyst selectivity ; Electrodes ; Electrolytic reduction ; Fossil fuels ; Microporosity

Ore Treatment:533.1 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Physical Properties of Gases, Liquids and Solids:931.2

2-s2.0-85064162190

Scopus

1.Department of ChemistryYale University,New Haven,06520,United States
2.Energy Sciences InstituteYale University,West Haven,06516,United States
3.Department of Materials Science and EngineeringShenzhen Key Laboratory of Printed Organic ElectronicsSouthern University of Science and Technology,Shenzhen,518055,China
4.Institute of Functional Nano and Soft MaterialsJiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow University,Suzhou,215123,China
5.EastChemSchool of ChemistryUniversity of Edinburgh,Edinburgh,EH9 3FJ,United Kingdom

Lu，Xu,Jiang，Zhan,Yuan，Xiaolei,et al. A bio-inspired O 2 -tolerant catalytic CO 2 reduction electrode[J]. Science Bulletin,2019,64(24):1890-1895.

Lu，Xu.,Jiang，Zhan.,Yuan，Xiaolei.,Wu，Yueshen.,Malpass-Evans，Richard.,...&Wang，Hailiang.(2019).A bio-inspired O 2 -tolerant catalytic CO 2 reduction electrode.Science Bulletin,64(24),1890-1895.

Lu，Xu,et al."A bio-inspired O 2 -tolerant catalytic CO 2 reduction electrode".Science Bulletin 64.24(2019):1890-1895.