Highly active oxygen evolution integrated with efficient CO2 to CO electroreduction

Meng，Yongtao1,2; Zhang，Xiao2,3; Hung，Wei Hsuan2,4; He，Junkai5; Tsai，Yi Sheng4; Kuang，Yun2; Kenney，Michael J.2; Shyue，Jing Jong6; Liu，Yijin7; Stone，Kevin H.7; Zheng，Xueli8; Suib，Steven L.5; Lin，Meng Chang1; Liang，Yongye3; Dai，Hongjie2

2019-11-26

10.1073/pnas.1915319116

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA   影响因子和分区

0027-8424

1091-6490

Electrochemical reduction of CO to useful chemicals has been actively pursued for closing the carbon cycle and preventing further deterioration of the environment/climate. Since CO reduction reaction (CORR) at a cathode is always paired with the oxygen evolution reaction (OER) at an anode, the overall efficiency of electrical energy to chemical fuel conversion must consider the large energy barrier and sluggish kinetics of OER, especially in widely used electrolytes, such as the pH-neutral CO-saturated 0.5 M KHCO. OER in such electrolytes mostly relies on noble metal (Ir- and Ru-based) electrocatalysts in the anode. Here, we discover that by anodizing a metallic Ni–Fe composite foam under a harsh condition (in a low-concentration 0.1 M KHCO solution at 85 °C under a high-current ∼250 mA/cm), OER on the NiFe foam is accompanied by anodic etching, and the surface layer evolves into a nickel–iron hydroxide carbonate (NiFe-HC) material composed of porous, poorly crystalline flakes of flower-like NiFe layer-double hydroxide (LDH) intercalated with carbonate anions. The resulting NiFe-HC electrode in CO-saturated 0.5 M KHCO exhibited OER activity superior to IrO, with an overpotential of 450 and 590 mV to reach 10 and 250 mA/cm, respectively, and high stability for >120 h without decay. We paired NiFe-HC with a CORR catalyst of cobalt phthalocyanine/carbon nanotube (CoPc/CNT) in a CO electrolyzer, achieving selective cathodic conversion of CO to CO with >97% Faradaic efficiency and simultaneous anodic water oxidation to O. The device showed a low cell voltage of 2.13 V and high electricity-to-chemical fuel efficiency of 59% at a current density of 10 mA/cm

CO2 electrolyzer CO2 reduction Electrocatalysis Oxygen evolution PH-neutral electrolyte

SCI

英语

NI期刊

其他

Ministry of Science and Technology, Taiwan[MOST-106-2918-I-035-002]

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:000499101100014

NATL ACAD SCIENCES

BIOLOGY & BIOCHEMISTRY;CLINICAL MEDICINE;MULTIDISCIPLINARY;PLANT & ANIMAL SCIENCE;ENVIRONMENT/ECOLOGY;SOCIAL SCIENCES, GENERAL;MICROBIOLOGY;ECONOMICS BUSINESS;IMMUNOLOGY;MATERIALS SCIENCE;MATHEMATICS;SPACE SCIENCE;MOLECULAR BIOLOGY & GENETICS;PHARMACOLOGY & TOXICOLOGY;CHEMISTRY;PSYCHIATRY/PSYCHOLOGY;NEUROSCIENCE & BEHAVIOR;PHYSICS;GEOSCIENCES;AGRICULTURAL SCIENCES;ENGINEERING

2-s2.0-85075494460

Scopus

1.College of Electrical Engineering and Automation,Shandong University of Science and Technology,Qingdao,266590,China
2.Department of Chemistry,Stanford University,Stanford,94305,United States
3.Department of Materials Science and Engineering,South University of Science and Technology of China,Shenzhen,518055,China
4.Institute of Materials Science and Engineering,National Central University,Taoyuan,32001,Taiwan
5.Institute of Materials Science,University of Connecticut,Storrs,06269,United States
6.Research Center of Applied Science,Academia Sinica,Taipei,115,Taiwan
7.Stanford Synchrotron Radiation Light Source,SLAC National Accelerator Laboratory,Menlo Park,94025,United States
8.Department of Material Science and Engineering,Stanford University,Stanford,94305,United States

Meng，Yongtao,Zhang，Xiao,Hung，Wei Hsuan,et al. Highly active oxygen evolution integrated with efficient CO2 to CO electroreduction[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2019,116(48):23915-23922.

Meng，Yongtao.,Zhang，Xiao.,Hung，Wei Hsuan.,He，Junkai.,Tsai，Yi Sheng.,...&Dai，Hongjie.(2019).Highly active oxygen evolution integrated with efficient CO2 to CO electroreduction.PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,116(48),23915-23922.

Meng，Yongtao,et al."Highly active oxygen evolution integrated with efficient CO2 to CO electroreduction".PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA 116.48(2019):23915-23922.