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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Iron-containing sulfur/nitrogen co-doped porous carbons via composite salt modification to promote the oxygen reduction catalysis

Chenyang Shu,Xinru Xu,Jianglin Chen,Hongdian Chen,Jinyan Wu,Rong Jin,Yao Liu,Chaozhong Guo,Chuanlan Xu,Yujun Si

Carbon materials with high micropore volume and great specific surface area (SSA) are developed as catalysts for oxygen reduction reaction. Sodium lignosulfonate was used as the primary starting material for effectively doping of iron and nitrogen using ferric chloride hexahydrate and melamine, capitalizing on its robust coordination characteristics. The influences of the magnesium oxide template and composite salt etching on the pore structure and catalytic performance are comprehensively investigated. Modulation of MgO template and composite salt during high-temperature pyrolysis produces the catalyst (Fe-NS-PC) with a hierarchical porous structure and a 1699 m 2  g −1 of specific surface area. It promotes the exposure of active sites, and mobility of reactants and products during oxygen reduction process. Thus, the Fe-NS-PC catalyst possess an oxygen reduction reaction (ORR) activity ( E 1/2  = 0.865 V vs . RHE) in alkaline medium, being similar to the Pt/C catalyst. In zinc-air battery (ZAB) testing, the specific energy density is reduced by 6% after ∼120 h of uninterrupted discharge when the negative zinc foil is substituted, demonstrating the exceptional stability. This work presents a practical guide for the subsequent modification of carbon materials using template and composite salts modification.

研究领域: 材料科学 · 催化化学 · 能源存储与转换
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

In situ exsolution-induced formation of amorphous/crystalline heterointerfaces in Ba0.6Sr0.4Co0.8Fe0.2O3-δ for enhanced oxygen electrocatalysis in zinc-air batteries

Zihao Xie,Qian Yang,Xiaomin Xu,Deqing He,Yongning Yi,Hao Qiu,Huangang Shi,Yingping Pang,Wei Wang,Chao Su

The main obstacle in the commercial application of aqueous zinc-air batteries (ZABs) are emerging viable, sustainable, and safe alternatives in electrochemical energy conversion technologies. However, the practical realization of ZABs is impeded by four-electron oxygen evolution (OER) and reduction reactions (ORR) and their sluggish kinetics. Herein, we propose a niobium and fluorine co-doping strategy to regulate in situ Ba and Sr exsolution, inducing the formation of amorphous/crystalline Ba 0.6 Sr 0.4 Co 0.8 Fe 0.2 O 3-δ heterointerfaces with an alkali treatment. Associated with the formation of a low valence state of cobalt, an abundant oxygen defects, and amorphous/crystalline feature, the catalyst enables enhanced oxygen binding energy in the OER and ORR activities. The optimized bifunctional perovskite oxide (BSCFeN-F al ) catalysts present an excellent oxygen electrocatalytic activity and stability, with much lower OER and ORR overpotentials than other perovskite oxides in this work and with negligible performance decay in accelerated durability testing. When used as an air-electrode, the BSCFeN-F al demonstrates excellent performance, achieving high power density and remarkable cycling stability. This work highlights the essential function of the heterostructure interface in oxygen electrocatalysis, opening a new avenue to advanced neutral metal-air batteries.

研究领域: 材料科学 · 电化学 · 能源技术
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Materials · 2025 ·Vol. 18 ·期 10 ·2251 · IF 3.2

Structural Engineering of Bimetallic CoCe-ZIF Derives Catalysts with Optimized Electronic Structure for Enhanced Oxygen Electrocatalysis

Linxiang Zhou,Chaoyang Shi,Huaqi Wang,Danyang Wei,Haodong Jin,Haoqi Li,Zhiwei Meng,Mingli Xu

Developing efficient and durable non-precious metal catalysts for oxygen electrocatalysis in fuel cells and zinc–air batteries remains an urgent issue to be addressed. Herein, a bimetallic CoCe-NC catalyst is synthesized through pyrolysis of Co/Ce co-doped metal–organic frameworks (MOFs), retaining the inherently high surface area of MOFs to maximize the exposure of Co-N and Ce-N active sites. The electronic interaction between Co and Ce atoms effectively modulates the adsorption/desorption behavior of oxygen-containing intermediates, thereby enhancing intrinsic catalytic activity. In alkaline media, the CoCe-NC catalyst exhibits E1/2= 0.854 V electrocatalytic capability comparable to commercial Pt/C, along with superior methanol resistance and durability. Notably, CoCe-NC demonstrates an overpotential 84 mV lower than Pt/C at 300 mA cm−2in a GDE half-cell. When the catalyst is employed as a cathode in zinc–air batteries, it demonstrates an open-circuit voltage of 1.47 V, a peak power density of 202 mW cm−2, and exceptional cycling durability.

研究领域: 材料科学 · 电化学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2025 · IF 3.9

Carbon Nanotube-Loaded NiCo2O4 Nanoparticles Boosting Oxygen Electrocatalysis in Zinc–Air Batteries

Tao Cong,Xiaoyu Wang,Xifeng Ding

Metal–air batteries, with high energy density and eco-friendliness, are crucial for sustainable energy. Although abundant and low-cost, spinel oxides, ideal for metal–air batteries, suffer from low conductivity, hindering electron transport and slowing electrocatalytic kinetics. In this work, NiCo2O4 (NCO) was embedded on carbon nanotubes (CNTs) via a hydrothermal method to form a composite catalyst (NCO-1CNTs), and subsequent annealing in nitrogen enhanced oxygen vacancy concentration in the spinel structure. In 0.1 M KOH, NCO-1CNTs achieves outstanding oxygen evolution reaction (OER) performance (η10 = 427 mV) and oxygen reduction reaction (ORR) performance (jL = 5.1 mA cm–2), surpassing NCO by 16.6% and 82.1%. The enhanced catalytic activity is attributed to the high conductivity of carbon nanotubes, which accelerates electron transfer. Additionally, carbon nanotubes prevent spinel oxide aggregation, increase active sites, and form a porous structure, enhancing oxygen species transport. Moreover, annealing NCO-1CNTs in a nitrogen atmosphere induces the spinel component to generate more oxygen vacancies, boosting catalytic performance. The resulting zinc–air battery delivers a power density of 68 mW cm–2 and exhibits stable performance over 100 h of charge–discharge cycling. This study delivers a low-cost, high-activity, stable bifunctional cathode catalyst, signaling great promise for commercial rechargeable zinc–air batteries.

研究领域: 材料科学 · 电化学 · 能源技术
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Breaking the trade-off: Janus gel empowers flexible Zn-air batteries with simultaneous ultrahigh strength and ionic flux

Xiaohong Sun,Jinhui Zhang,Xueyan Li,Qinglu Peng,Xuliang Yang,Qingju Liu,Longzhou Zhang

The inherent trade-off between mechanical robustness and ionic transport efficiency in gel electrolytes has posed a long-standing challenge for advancing solid-state zinc-air batteries. Conventional approaches struggle to reconcile micron-scale pores (essential for mechanical reinforcement) with macroporous networks (critical for rapid ion migration). In this study, a novel strategy was employed to introduce micropores onto the skeleton of a macroporous gel. The X-ray tomography reveals this secondary structure for the first time. The zinc-air battery assembled by this gel exhibit the high ion conductivity of 205 mS cm −1 and undertake a stress of 984 Kpa. Additionally, the lifetimes of button cell and flexible Zinc-air battery reach 120 h and 97 h respectively.

CAS / MDL: 110-26-9 7727-21-1
研究领域: 材料科学 · 能源工程
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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 44 ·期 29 ·12850-12856 · IF 3.288

Porous carbons embedded with nitrogen-coordinated cobalt as an exceptional electrochemical catalyst for high-performance Zn–air batteries

Shice Wei,Fan Zhang,Zhenying Chen,Junjie Ding,Bai Xue,Chenbao Lu

The development of non-noble, efficient, and durable catalysts to replace expensive Pt-based catalysts for boosting the oxygen reduction reaction (ORR) is always an imperative and challenging topic. Herein, a triazine-linked covalent framework was prepared by using a cobalt-centered porphyrin derivative via a facile ionothermal approach, which was readily converted to a series of porous carbons (termed Co/N-PCs) with high surface areas upon controlled thermal treatment. The cobalt atoms coordinated with nitrogen were uniformly dispersed within the resulting porous structures. Accordingly, such as-prepared Co/N-PCs exhibited high activity for the ORR with a positive onset potential of 0.91 V (vs. RHE) and half-wave potential of 0.83 V, as well as good methanol tolerance and long-time durability. When used as air cathodes for Zn–air batteries, high power density (158.9 mW cm−2) and specific capacity (797 mA h g−1) were achieved, outperforming commercial Pt/C.

研究领域: 材料科学 · 电化学 · 能源科学
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Journal of Materials Chemistry A · 2019 ·Vol. 7 ·期 37 ·21232-21243 · IF 10.733

Electronic reconfiguration of Co2P induced by Cu doping enhancing oxygen reduction reaction activity in zinc–air batteries

Lechen Diao,Tao Yang,Biao Chen,Biao Zhang,Naiqin Zhao,Chunsheng Shi,Enzuo Liu,Liying Ma,Chunnian He

Developing highly efficient and low-cost bifunctional electrocatalysts towards the oxygen reduction reaction (ORR) is important for Zn–air batteries (ZABs) but still a challenge. In this work, electronic reconfiguration and structural optimization are simultaneously conducted to enhance the oxygen reduction reaction (ORR) electrocatalytic activity of Co2P nanoparticles, which were doped with Cu and confined within 2D ultrathin N,P-codoped carbon (NPC) nanosheets. Density functional theory calculations reveal that Cu doping can lead to more positive sites at the neighbouring Co site and weaken the binding force between the surface active sites and the adsorbed intermediates, while the 2D ultrathin nanosheets with Cu doped Co2P nanoparticles tightly anchored can remarkably boost the surface exposure of actives sites endowing such an architecture with efficient mass and charge transport pathways. As expected, the optimized Cu doped Co2P on 2D ultrathin N,P-codoped carbon (Cu-Co2P@2D-NPC) with 7.1% Cu doping exhibits a higher half-wave potential of 0.835 V than Pt/C (0.830 V). Meanwhile, flexible solid state ZABs assembled based on the 7.1%Cu-Co2P@2D-NPC hybrid deliver a high power density of 52.5 mW cm−2 and 32 h stability in the flat and folded states. This promising work holds significant potential to fabricate an efficient electrocatalyst for flexible solid state ZABs and further understand the relationship between the structure and activity.

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

γ-Fe2O3 clusters embedded in 1D porous N-doped carbon matrix as pH-universal electrocatalyst for enhanced oxygen reduction reaction

Zhihui Yao,Yuting Li,Daisong Chen,Yiwen Zhang,Xinghong Bao,Juan Wang,Qin Zhong

Carbon-based materials have shown promising results in replacing commercial Pt/C as highly efficient oxygen reduction reaction (ORR) catalysts in renewable energy devices. Designing unique structures of carbon matrix and introducing more active sites are essential for their application as electrode materials. Herein, a feasible approach is reported to synthesize dispersive γ -Fe 2 O 3 clusters embedded in 1D porous carbon nanofibers (CNFs) ( γ -Fe 2 O 3 @CNFs-12) through electrospinning, impregnation and pyrolysis processes. The resulted γ -Fe 2 O 3 @CNFs-12 exhibits excellent ORR performance in alkaline electrolyte with a surprising half-wave potential ( E 1/2 ) of 0.905 V and merely 5 mV drop of the potential after 5000 cycles, outperforming that of commercial Pt/C. Meanwhile, it also shows considerable ORR performance in acidic and neutral media. The remarkable ORR catalytic activity and durability are primarily attributable to the well-designed 1D hierarchical porous structure and accessible γ -Fe 2 O 3 clusters that embedded in carbon nanofibers. γ -Fe 2 O 3 @CNFs-12 is also capable to act as an air cathode for Zn-air batteries with an open circuit voltage of 1.428 V. This work provides a new perspective to the novel design and synthesis of carbon-based ORR electrocatalysts.

CAS / MDL: 693-98-1
研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Lithium-Induced Oxygen Vacancies in MnO2@MXene for High-Performance Zinc–Air Batteries

Qing Sun,Ziyang Guo,Tie Shu,Yongfei Li,Kailin Li,Yuxin Zhang,Liang Li,Jiaoyi Ning,Ke Xin Yao

The traditional methods for creating oxygen vacancies in materials present several challenges and limitations, such as high preparation temperatures, limited oxygen vacancy generation, and morphological destruction, which hinder the application of transition metal oxides in the field of zinc–air batteries (ZABs). In order to address these limitations, we have introduced a pioneering lithium reduction strategy for generating oxygen vacancies in δ-MnO2@MXene composite materials. This strategy stands out for its simplicity of implementation, applicability at room temperature, and preservation of the material’s structural integrity. This research demonstrates that aqueous Ov-MnO2@MXene-5, with introduced oxygen vacancies, exhibits an outstanding oxygen reduction reaction (ORR) activity with an ORR half-wave potential reaching 0.787 V. DFT calculations have demonstrated that the enhanced activity could be attributed to adjustments in the electronic structure and alterations in adsorption bond lengths. These adjustments result from the introduction of oxygen vacancies, which in turn promote electron transport and catalytic activity. In the context of zinc–air batteries, cells with Ov-MnO2@MXene-5 as the air cathode exhibit outstanding performance, featuring a significantly improved maximum power density (198.3 mW cm–2) and long-term cycling stability. Through the innovative strategy of introducing oxygen vacancies, this study has successfully enhanced the electrochemical catalytic performance of MnO2, overcoming the limitations associated with traditional methods for creating oxygen vacancies. Consequently, this research opens up new avenues and directions for nonprecious metal catalyst application in ZABs.

研究领域: 材料科学 · 电化学 · 能源存储与转换
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

All-in-one and bipolar-membrane-free acid-alkaline hydrogel electrolytes for flexible high-voltage Zn-air batteries

Siyuan Zhao,Tong Liu,Yawen Dai,Yang Wang,Zengjia Guo,Shuo Zhai,Jie Yu,Chunyi Zhi,Meng Ni

The low operating voltage of 1.4 V limits the widespread application of flexible Zn-air batteries (ZABs) in wearable electronics. However, a high-voltage flexible ZAB has not been achieved yet, which results from the few choices of fitted flexible electrolytes.   Now we propose a novel, universal, and simple strategy to design all-in-one and membrane-free acid-alkaline flexible electrolytes based on thermo-reversible Pluronic® F127 hydrogels. Benefiting from the unique sol–gel transition property of Pluronic® F127 hydrogel, the acid and alkaline can be decoupled but integrated simultaneously in one hydrogel.   Surprisingly,   the as-developed ZAB   achieves   an unprecedentedly high voltage of 2 V, surpassing all the existing flexible ZABs.   Meanwhile, this battery exhibits remarkable high-voltage stability of 37 h and a large area capacity   of 1.35 mAh cm −2 without the use of costly bipolar membranes. Our work presents a pioneering example for flexible high-voltage ZAB and may further inspire other designs of flexible high-voltage aqueous batteries and decoupled dual-electrolyte batteries.

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 能源技术 · 化学工程
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Carbon Energy · 2022 ·Vol. 4 ·期 5 ·762-775 · IF 21.556

Facile carbon cloth activation strategy to boost oxygen reduction reaction performance for flexible zinc-air battery application

Revanasiddappa Manjunatha,Jingchao Yuan,Li Hongwei,Shu-Qi Deng,Ejikeme R. Ezeigwe,Yinze Zuo,Li Dong,Aijun Li,Wei Yan,Fangzhou Zhang,Jiujun Zhang

Flexible and all-solid-state zinc-air batteries (ZABs) are highly useful and also in demand due to their theoretical high energy densities and special applications. The limitation in their performance arises due to their catalyst-coated cathode electrodes in terms of catalytic activity and stability as well as cost. In this paper, a novel and environmentally friendly activation strategy is developed to activate the carbon cloth (CC) for the electrodes. The activated CC serves as a catalyst-free air cathode with high conductivity, excellent mechanical strength, and flexibility, in addition to low cost. The strategy is performed by simply electro-oxidizing and electroreducing CC under ultrahigh direct current (DC) voltage in a diluted NH 4 Cl aqueous electrolyte. It is found that the electro-oxidation not only results in the formation of a graphene-like exfoliated carbon layer on the surface of CC but also induces the incorporation of oxygen-containing groups and doping of nitrogen and chloride atoms. After the electroreduction, the π-conjugated carbon network of CC is partially restored, leading to the recovery of electroconductivity. Such an electroactivated CC shows excellent oxygen reduction reaction activity. The aqueous flexibility and all-solid-state ZABs are assembled using such an electroactivated CC cathode without any catalyst loading. Both ZABs can achieve good durability and deliver high peak power density and an energy density as high as 690 Wh kg −1 , demonstrating the excellent potential of this electroactivated CC in practical devices.

研究领域: 材料科学 · 能源技术 · 环境科学
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2022 · IF 10.319

Tellurium intervened Fe-N codoped carbon for improved oxygen reduction reaction and high-performance Zn-air batteries

Rui Wang,Zihan Meng,Xuemin Yan,Tian Tian,Ming Lei,Rami Adel Pashameah,Hala M. Abo-Dief,Hassan Algadi,Nina Huang,Zhanhu Guo,Haolin Tang

Pyrolysis-acquired iron and nitrogen codoped carbon (Fe-N-C) has been comprehensively investigated for its promising oxygen reduction reaction (ORR) catalytic performance and structural complexity. The modification of non-metal elements with larger atomic radius and the corresponding intrinsic microstructure-property relations are rarely reported. In this study, tellurium (Te) intervened Fe-N-C was prepared by micelles-induced polymerization with Te nanowires as an in-situ intervening agent. The out-plane bonding of Te with Fe induced the increase of both N content and proportion of pyridinic N on the material surface, thus improving the ORR catalytic performance. The assembled Zn-air battery demonstrated a maximum power density of 250 mW/cm 2 and excellent rate capability under various discharge current densities, which was much better than the Pt/C. Overall, the current work demonstrates a novel Te/Fe-N-C material and reveals an original Te intervened Fe-N-C strategy and N reconfiguration mechanism, which is of great significance for the design of key materials in energy-related fields.

研究领域: 材料科学 · 电化学 · 能源科学
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