Asymmetric Co-N3P1 Trifunctional Catalyst with Tailored Electronic Structures Enabling Boosted Activities and Corrosion Resistance in an Uninterrupted Seawater Splitting System

Wang，Xingkun1; Zhou，Xinkun2; Li，Cheng3,4; Yao，Hanxu1,2; Zhang，Canhui1; Zhou，Jian1; Xu，Ren1; Chu，Lei1; Wang，Huanlei1; Gu，Meng3; Jiang，Heqing2; Huang，Minghua1

2022

10.1002/adma.202204021

ADVANCED MATERIALS   Impact Factor & Quartile

0935-9648

1521-4095

Employing seawater splitting systems to generate hydrogen can be economically advantageous but still remains challenging, particularly for designing efficient and high Cl-corrosion resistant trifunctional catalysts toward the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). Herein, single Co-N-C catalysts with well-defined symmetric Co-N sites are selected as atomic platforms for electronic structure tailoring. Density function theory reveals that P-doping into Co-N-C can lead to the formation of asymmetric Co-NP sites with symmetry-breaking electronic structures, enabling the affinity of strong oxygen-containing intermediates, moderate H adsorption, and weak Cl adsorption. Thus, ORR/OER/HER activities and stability are optimized simultaneously with high Cl-corrosion resistance. The asymmetric Co-NP structure based catalyst with boosted ORR/OER/HER performance endows seawater-based Zn–air batteries (S-ZABs) with superior long-term stability over 750 h and allows seawater splitting to operate continuously for 1000 h. A self-driven seawater splitting powered by S-ZABs gives ultrahigh H production rates of 497 µmol h. This work is the first to advance the scientific understanding of the competitive adsorption mechanism between Cl and reaction intermediates from the perspective of electronic structure, paving the way for synthesis of efficient trifunctional catalysts with high Cl-corrosion resistance.

asymmetric Co–N 3P 1 sites electronic structure H 2 production rates high Cl −-corrosion resistance trifunctional catalysts

SCI ; EI

English

NI Journal Papers

Corresponding

National Natural Science Foundation of China[21775142] ; Key Research & Development Project of Shandong (Major Innovation Projects)[2019JZZY010905] ; Natural Science Foundation of Shandong Province[ZR2020ZD10] ; Shenzhen Natural Science Fund[20200925154115001] ; Shenzhen Fundamental Research Funding["JCYJ20210324115809026","JCYJ20200109141216566"]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000844123300016

WILEY-V C H VERLAG GMBH

20223012402230

Adsorption ; Corrosion resistance ; Density functional theory ; Electrolytic reduction ; Electronic structure ; Hydrogen production ; Oxygen ; Probability density function ; Proton exchange membrane fuel cells (PEMFC) ; Reaction intermediates ; Seawater corrosion

Seawater, Tides and Waves:471.4 ; Gas Fuels:522 ; Ore Treatment:533.1 ; Metals Corrosion:539.1 ; Fuel Cells:702.2 ; Chemical Reactions:802.2 ; Chemical Operations:802.3 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

MATERIALS SCIENCE

2-s2.0-85134610481

Scopus

1.School of Materials Science and Engineering,Ocean University of China,Qingdao,266100,China
2.Qingdao Key Laboratory of Functional Membrane Material and Membrane Technology,Qingdao Institute of Bioenergy and Bioprocess Technology,Chinese Academy of Sciences,Qingdao,266101,China
3.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
4.School of Physics and Astronomy,University of Birmingham,Birmingham,B15 2TT,United Kingdom

Wang，Xingkun,Zhou，Xinkun,Li，Cheng,et al. Asymmetric Co-N3P1 Trifunctional Catalyst with Tailored Electronic Structures Enabling Boosted Activities and Corrosion Resistance in an Uninterrupted Seawater Splitting System[J]. ADVANCED MATERIALS,2022,34(34).

Wang，Xingkun.,Zhou，Xinkun.,Li，Cheng.,Yao，Hanxu.,Zhang，Canhui.,...&Huang，Minghua.(2022).Asymmetric Co-N3P1 Trifunctional Catalyst with Tailored Electronic Structures Enabling Boosted Activities and Corrosion Resistance in an Uninterrupted Seawater Splitting System.ADVANCED MATERIALS,34(34).

Wang，Xingkun,et al."Asymmetric Co-N3P1 Trifunctional Catalyst with Tailored Electronic Structures Enabling Boosted Activities and Corrosion Resistance in an Uninterrupted Seawater Splitting System".ADVANCED MATERIALS 34.34(2022).