Molecular design and coordination regulation of atomically dispersed bi-functional catalysts for oxygen electrocatalysis

Sheng, Kuang; Li, Guang; Hao, Jiayu; Wang, Yanqiu; Kaili, Shi; Liu, Yang; Zhang, Ning; Qiu, Xiaoqing; Liu, Min; Li, Wenzhang; Li, Jie

doi:10.1039/d2ta09788e

J. Mater. Chem. A

2023

DOI: 10.1039/d2ta09788e

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Molecular design and coordination regulation of atomically dispersed bi-functional catalysts for oxygen electrocatalysis

Kuang Sheng

Guang Li

Jiayu Hao

et al.

Abstract: Oxygen reduction (ORR) and evolution reaction (OER) play important roles in new sustainable energy conversion devices to address the dilemma of energy shortage, but are limited by slow electrochemical kinetic...

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2024

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Cited by 7 publications

(1 citation statement)

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“…The traditional fossil energy system is unable to meet the vision of sustainable social development due to a series of inherent shortcomings such as limited resources, non-renewable, and environmental pollution. [1][2][3] Therefore, many researchers in various countries have been working on finding alternatives to solve the energy crisis. As a "green renewable energy technology," metal-air batteries have attracted great interest for their low cost, high safety, environmental benignity, high specific capacity, and good stability in aqueous electrolytes.…”

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confidence: 99%

Heteroatom Sulfur-Modified ZIF-8 Derived Zn, N Co-Doped Carbon Nanocages as Highly Efficient ORR Catalysts for Zn-Air Batteries

Li,

Tang,

Sheng

et al. 2024

J. Electrochem. Soc.

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Carbon-based electrocatalysts derived from zeolitic imidazolate framework-8 (ZIF-8) have garnered significant attention, owing to their structural advantages, high surface area, and tunable active sites. Herein, we report the synthesis of heteroatom sulfur (S) modified ZIF-8 derived carbon nanocages (ZnS@N/S-C) for oxygen electrocatalysis through self-assembly and two-step pyrolysis. The resultant ZnS@N/S-C exhibits catalytic activity towards oxygen reduction reaction (ORR) with high half-wave potential (0.86 V) and stability (91.4%), separately, which is comparable to or superior to Pt/C. Furthermore, the application of ZnS@N/S-C as a cathode for Zn-air batteries (ZABs) demonstrates performance metrics such as an open-circuit voltage of 1.407 V, a power density of 114.4 mW cm-2, and a specific capacity of 764.6 mAh gZn-1, etc. surpassing Pt/C. The performance of ZnS@N/S-C can be attributed to the fact that the introduction of S significantly increases the specific surface area, pore volume, and defect extent of the catalyst, while optimizing the electronic structure and generating ZnS active nanocrystals. This work employs a simple sulfurization strategy to enhance the ORR activity of ZIF-8-derived Zn-based catalysts with fully filled 3d orbitals, providing guidance for the development of such materials.

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confidence: 99%

Heteroatom Sulfur-Modified ZIF-8 Derived Zn, N Co-Doped Carbon Nanocages as Highly Efficient ORR Catalysts for Zn-Air Batteries

Li,

Tang,

Sheng

et al. 2024

J. Electrochem. Soc.

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Hetero‐Diatomic CoN₄‐NiN₄ Site Pairs with Long‐Range Coupling as Efficient Bifunctional Catalyst for Rechargeable Zn–Air Batteries

Yang,

Li,

Liang

et al. 2024

Advanced Science

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In this study, Co/Ni‐NC catalyst with hetero‐diatomic Co/Ni active sites dispersed on nitrogen‐doped carbon matrix is synthesized via the controlled pyrolysis of ZIF‐8 containing Co2+ and Ni2+ compounds. Experimental characterizations and theoretical calculations reveal that Co and Ni are atomically and uniformly dispersed in pairs of CoN4‐NiN4 with an intersite distance ≈0.41 nm, and there is long‐range d–d coupling between Co and Ni with more electron delocalization for higher bifunctional activity. Besides, the in situ grown carbon nanotubes at the edges of the catalyst particles allow high electronic conductivity for electrocatalysis process. Electrochemical evaluations demonstrate the superior ORR and OER bifunctionality of Co/Ni‐NC catalyst with a narrow potential gap of only 0.691 V and long‐term durability, significantly prevailing over the single‐atom Co‐NC and Ni‐NC catalysts and the benchmark Pt/C and RuO2 catalysts. Co/Ni‐NC catalyzed Zn–air batteries achieve a high specific capacity of 771 mAh g−1 and a long continuous operation period up to 340 h with a small voltage gap of ≈0.65 V, also much superior to Pt/C‐RuO2.

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Fe, N, S co-doped carbon network derived from acetate-modified Fe-ZIF-8 for oxygen reduction reaction

Zhang,

Deng,

Bai

et al. 2024

Journal of Colloid and Interface Science

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Molecular design and coordination regulation of atomically dispersed bi-functional catalysts for oxygen electrocatalysis

Abstract: Oxygen reduction (ORR) and evolution reaction (OER) play important roles in new sustainable energy conversion devices to address the dilemma of energy shortage, but are limited by slow electrochemical kinetic...

Cited by 7 publications

References 168 publications

Heteroatom Sulfur-Modified ZIF-8 Derived Zn, N Co-Doped Carbon Nanocages as Highly Efficient ORR Catalysts for Zn-Air Batteries

Heteroatom Sulfur-Modified ZIF-8 Derived Zn, N Co-Doped Carbon Nanocages as Highly Efficient ORR Catalysts for Zn-Air Batteries

Hetero‐Diatomic CoN₄‐NiN₄ Site Pairs with Long‐Range Coupling as Efficient Bifunctional Catalyst for Rechargeable Zn–Air Batteries

Fe, N, S co-doped carbon network derived from acetate-modified Fe-ZIF-8 for oxygen reduction reaction

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Molecular design and coordination regulation of atomically dispersed bi-functional catalysts for oxygen electrocatalysis

Abstract: Oxygen reduction (ORR) and evolution reaction (OER) play important roles in new sustainable energy conversion devices to address the dilemma of energy shortage, but are limited by slow electrochemical kinetic...

Cited by 7 publications

References 168 publications

Heteroatom Sulfur-Modified ZIF-8 Derived Zn, N Co-Doped Carbon Nanocages as Highly Efficient ORR Catalysts for Zn-Air Batteries

Heteroatom Sulfur-Modified ZIF-8 Derived Zn, N Co-Doped Carbon Nanocages as Highly Efficient ORR Catalysts for Zn-Air Batteries

Hetero‐Diatomic CoN4‐NiN4 Site Pairs with Long‐Range Coupling as Efficient Bifunctional Catalyst for Rechargeable Zn–Air Batteries

Fe, N, S co-doped carbon network derived from acetate-modified Fe-ZIF-8 for oxygen reduction reaction

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Hetero‐Diatomic CoN₄‐NiN₄ Site Pairs with Long‐Range Coupling as Efficient Bifunctional Catalyst for Rechargeable Zn–Air Batteries