Heteroatom-Driven Coordination Fields Altering Single Cerium Atom Sites for Efficient Oxygen Reduction Reaction

Leilei Yin; Shuai Zhang; Mingzi Sun; Siyuan Wang; Bolong Huang; Yaping Du

doi:10.1002/adma.202302485

Heteroatom-Driven Coordination Fields Altering Single Cerium Atom Sites for Efficient Oxygen Reduction Reaction

Leilei Yin
, Shuai Zhang
, Mingzi Sun
, Siyuan Wang
, Bolong Huang^*
, Yaping Du^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

216 Citations (Scopus)

Abstract

For current single-atom catalysts (SACs), modulating the coordination environments of rare-earth (RE) single atoms with complex electronic orbital and flexible chemical states is still limited. Herein, cerium (Ce) SAs supported on a P, S, and N co-doped hollow carbon substrate (Ce SAs/PSNC) for the oxygen reduction reaction (ORR) are reported. The as-prepared Ce SAs/PSNC possesses a half-wave potential of 0.90 V, a turnover frequency value of 52.2 s⁻¹ at 0.85 V, and excellent stability for the ORR, which exceeds the commercial Pt/C and most recent SACs. Ce SAs/PSNC-based liquid zinc–air batteries (ZABs) exhibit a high and stable open-circuit voltage of 1.49 V and a maximum power density of 212 mW cm⁻². As the catalyst of the air cathode, it also displays remarkable performance in flexible electronic devices. Theoretical calculations reveal that the introduction of S and P sites induces significant electronic modulations to the Ce SA active sites. The P and S dopings promote the electroactivity of Ce SAs and improve the overall site-to-site electron transfer within the Ce SAs/PSNC. This work offers a unique perspective for modulating RE-based SACs in a complex coordination environment toward superior electrocatalysis and broad applications in energy conversion and storage devices. © 2023 Wiley-VCH GmbH.

Original language	English
Article number	2302485
Journal	Advanced Materials
Volume	35
Issue number	28
Online published	24 May 2023
DOIs	https://doi.org/10.1002/adma.202302485
Publication status	Published - 13 Jul 2023
Externally published	Yes

Funding

The authors acknowledge the support from the National Key R&D Program of China (2021YFA1501101), the National Natural Science Foundation of China (21971117), the National Natural Science Foundation of China/Research Grant Council of Hong Kong Joint Research Scheme (N_PolyU502/21), Functional Research Funds for the Central Universities, Nankai University (63186005), Tianjin Key Lab for Rare Earth Materials and Applications (ZB19500202), the funding for Projects of Strategic Importance of The Hong Kong Polytechnic University (Project Code: 1-ZE2V), Shenzhen Fundamental Research Scheme-General Program (JCYJ20220531090807017), 111 Project (No. B18030) from China, the Outstanding Youth Project of Tianjin Natural Science Foundation (20JCJQJC00130), Departmental General Research Fund (Project Code: ZVUL) of The Hong Kong Polytechnic University, the Key Project of Tianjin Natural Science Foundation (20JCZDJC00650), the National Postdoctoral Program for Innovative Talents (BX20220157), Open Foundation of State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures (Grant No. 2022GXYSOF7), Natural Science Foundation of Guangdong Province (2023A1515012219) and Haihe Laboratory of Sustainable Chemical Transformations. B.H. also thanks the support from Research Centre for Carbon-Strategic Catalysis (RC-CSC), Research Institute for Smart Energy (RISE), and Research Institute for Intelligent Wearable Systems (RI-IWEAR) of the Hong Kong Polytechnic University.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Research Keywords

coordination modulation
heteroatom doping
oxygen reduction reaction
rare-earth elements
single-atom catalyst

RGC Funding Information

RGC-funded

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10.1002/adma.202302485

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title = "Heteroatom-Driven Coordination Fields Altering Single Cerium Atom Sites for Efficient Oxygen Reduction Reaction",

abstract = "For current single-atom catalysts (SACs), modulating the coordination environments of rare-earth (RE) single atoms with complex electronic orbital and flexible chemical states is still limited. Herein, cerium (Ce) SAs supported on a P, S, and N co-doped hollow carbon substrate (Ce SAs/PSNC) for the oxygen reduction reaction (ORR) are reported. The as-prepared Ce SAs/PSNC possesses a half-wave potential of 0.90 V, a turnover frequency value of 52.2 s−1 at 0.85 V, and excellent stability for the ORR, which exceeds the commercial Pt/C and most recent SACs. Ce SAs/PSNC-based liquid zinc–air batteries (ZABs) exhibit a high and stable open-circuit voltage of 1.49 V and a maximum power density of 212 mW cm−2. As the catalyst of the air cathode, it also displays remarkable performance in flexible electronic devices. Theoretical calculations reveal that the introduction of S and P sites induces significant electronic modulations to the Ce SA active sites. The P and S dopings promote the electroactivity of Ce SAs and improve the overall site-to-site electron transfer within the Ce SAs/PSNC. This work offers a unique perspective for modulating RE-based SACs in a complex coordination environment toward superior electrocatalysis and broad applications in energy conversion and storage devices. {\textcopyright} 2023 Wiley-VCH GmbH.",

keywords = "coordination modulation, heteroatom doping, oxygen reduction reaction, rare-earth elements, single-atom catalyst",

author = "Leilei Yin and Shuai Zhang and Mingzi Sun and Siyuan Wang and Bolong Huang and Yaping Du",

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month = jul,

day = "13",

doi = "10.1002/adma.202302485",

language = "English",

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issn = "0935-9648",

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TY - JOUR

T1 - Heteroatom-Driven Coordination Fields Altering Single Cerium Atom Sites for Efficient Oxygen Reduction Reaction

AU - Yin, Leilei

AU - Zhang, Shuai

AU - Sun, Mingzi

AU - Wang, Siyuan

AU - Huang, Bolong

AU - Du, Yaping

PY - 2023/7/13

Y1 - 2023/7/13

N2 - For current single-atom catalysts (SACs), modulating the coordination environments of rare-earth (RE) single atoms with complex electronic orbital and flexible chemical states is still limited. Herein, cerium (Ce) SAs supported on a P, S, and N co-doped hollow carbon substrate (Ce SAs/PSNC) for the oxygen reduction reaction (ORR) are reported. The as-prepared Ce SAs/PSNC possesses a half-wave potential of 0.90 V, a turnover frequency value of 52.2 s−1 at 0.85 V, and excellent stability for the ORR, which exceeds the commercial Pt/C and most recent SACs. Ce SAs/PSNC-based liquid zinc–air batteries (ZABs) exhibit a high and stable open-circuit voltage of 1.49 V and a maximum power density of 212 mW cm−2. As the catalyst of the air cathode, it also displays remarkable performance in flexible electronic devices. Theoretical calculations reveal that the introduction of S and P sites induces significant electronic modulations to the Ce SA active sites. The P and S dopings promote the electroactivity of Ce SAs and improve the overall site-to-site electron transfer within the Ce SAs/PSNC. This work offers a unique perspective for modulating RE-based SACs in a complex coordination environment toward superior electrocatalysis and broad applications in energy conversion and storage devices. © 2023 Wiley-VCH GmbH.

AB - For current single-atom catalysts (SACs), modulating the coordination environments of rare-earth (RE) single atoms with complex electronic orbital and flexible chemical states is still limited. Herein, cerium (Ce) SAs supported on a P, S, and N co-doped hollow carbon substrate (Ce SAs/PSNC) for the oxygen reduction reaction (ORR) are reported. The as-prepared Ce SAs/PSNC possesses a half-wave potential of 0.90 V, a turnover frequency value of 52.2 s−1 at 0.85 V, and excellent stability for the ORR, which exceeds the commercial Pt/C and most recent SACs. Ce SAs/PSNC-based liquid zinc–air batteries (ZABs) exhibit a high and stable open-circuit voltage of 1.49 V and a maximum power density of 212 mW cm−2. As the catalyst of the air cathode, it also displays remarkable performance in flexible electronic devices. Theoretical calculations reveal that the introduction of S and P sites induces significant electronic modulations to the Ce SA active sites. The P and S dopings promote the electroactivity of Ce SAs and improve the overall site-to-site electron transfer within the Ce SAs/PSNC. This work offers a unique perspective for modulating RE-based SACs in a complex coordination environment toward superior electrocatalysis and broad applications in energy conversion and storage devices. © 2023 Wiley-VCH GmbH.

KW - coordination modulation

KW - heteroatom doping

KW - oxygen reduction reaction

KW - rare-earth elements

KW - single-atom catalyst

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U2 - 10.1002/adma.202302485

DO - 10.1002/adma.202302485

M3 - RGC 21 - Publication in refereed journal

SN - 0935-9648

VL - 35

JO - Advanced Materials

JF - Advanced Materials

IS - 28

M1 - 2302485

ER -

Heteroatom-Driven Coordination Fields Altering Single Cerium Atom Sites for Efficient Oxygen Reduction Reaction

Abstract

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Research Keywords

RGC Funding Information

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