INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Fengxian Zhang,Ye Chen,Yang Liu,Xupo Liu,Shuyan Gao
Constructing highly efficient and durable non-noble metal modified carbon catalysts for oxygen reduction reaction (ORR) in the whole pH range is essential for energy conversion devices but still remains a challenge. Herein, the Fe/Fe 3 C nanoparticles and Fe-N X species anchored on the interconnected mesoporous carbon materials are fabricated through an economical and facile template-assisted polymerization-pyrolysis strategy. The catalyst exhibits unique features with the electronic interaction between Fe/Fe 3 C and Fe−N X , large specific surface area and high mesoporous structure as well as nitrogen doping in porous carbon skeletons, which can effectively catalyze ORR over the full pH range. In an alkaline electrolyte , the optimized catalyst displays favorable ORR performance with positive onset potential ( E onset = 0.91 V), half-wave potential ( E 1/2 = 0.83 V), long-term cycles stability and methanol tolerance, exceeding those for the commercial Pt/C. Furthermore, the prepared catalyst could be directly assembled into the alkaline Zn−air battery that exhibits the open-circuit voltage of 1.44 V, high power density of 96.0 mW cm −2 and long-term durability. Therefore, the template-assisted polymerization-pyrolysis strategy provides a promising route for designing high-performance non-noble metal decorated ORR electrocatalysts .
研究领域:
材料科学
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电化学
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能源转换技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Na Li,Tingting Ma,Huihui Wang,Jiayi Li,Dingrong Qiu,Zhen Meng,Jiangdu Huang,Lijun Sui,Faming Han,Huidan Lu,Yongping Liu,Sundaram Chandrasekaran
Rational design of defected carbons adjacent to nitrogen (N) dopants is a fascinating but challenging approach for enhancing the catalytic performance of N-doped carbon. Meanwhile, the combined effect of heteroatom doping and defect engineering can efficiently increase the oxygen reduction reaction (ORR) ability of inactive carbons through charge redistribution. Herein, we report that an enhanced built-in electric field caused by the combined effect of N-doping and carbon defects in the two-dimensional (2D) mesoporous N-doped carbon nanoflakes (NCNF) is a promising technique for improving ORR performance. As a result, the NCNF exhibits more promising ORR activity than Pt/C and similar performance with reported robust catalysts. Comprehensive experimental and theoretical investigations suggest that topologically defected carbon adjacent to the graphitic valley nitrogen is a real active site, rendering optimal energy for the adsorption of ORR intermediates and lowering the total energy barrier for ORR. Also, NCNF-based Zn-air batteries exhibited an excellent power density and specific capacity of ∼121.10 mW cm −2 and ∼679.86 mA h g Zn −1 , respectively. This study not only offers new insights into defected carbons with graphitic valley N for ORR but also proposes novel catalyst design principles and provides a solid grasp of the built-in electric field effect on the ORR performance of defective catalysts.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2024
·Vol. 12
·期 1
·205-216
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IF 6.1
Tao-Tao Li,Yu-Rui Ji,Yi-Meng Wu,Peng-Fei Wang,Zong-Lin Liu,Jie Shu,Ting-Feng Yi
The electrocatalytic activity of catalysts can be significantly enhanced through the utilization of heterogeneous structures. Nevertheless, the optimization of both catalytic activity and durability via heterojunction engineering remains a considerable challenge. In this work, we fabricated electrocatalysts of Co/CoO heterojunctions on a highly porous hollow carbon material. The formation of heterojunctions increases the abundance of accessible active sites and optimizes the electrocatalytic reaction kinetics and reactivity. Thus, the prepared catalysts (Co/CoO@N–C-40) deliver robust and stable bifunctional oxygen electrocatalytic activity during the oxygen reduction/evolution reaction (ORR/OER) process. The performance of rechargeable zinc–air batteries (ZABs) greatly depends on bifunctional oxygen electrocatalysts, which are crucial for efficient charging and discharging processes. Consequently, the Co/CoO@N–C-40-based ZABs have superior cycling stability (750 h) and show a stable energy efficiency of 55.10% at 10 mA cm−2 (53.46% after 555 h). This work offers a high-quality oxygen electrocatalyst for ZABs and extends the application of heterogeneous interfacial catalysts in various energy storage and conversion devices.
研究领域:
材料科学
·
电化学
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能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2025
·
IF 3.9
Liu Qingye,Wang Chenghua,Zou Chang,Li Jiangtao,Liu Jun,Liu Yilun,Sun Xueyan,Zhao Wei
Polyvinyl alcohol (PVA) hydrogel as a hydrogel electrolyte faces issues such as fracture, dehydration, and poor conductivity, limiting its application in flexible zinc-air batteries. To address these, we propose a triethanolamine (TEA)-modified PVA-based hydrogel material (TPVA). TEA promoted formation of a uniform mesoporous structure and enables TPVA hydrogel to exhibit excellent mechanical properties, with an elongation at break (425%) approximately twice that of PVA (230%). Additionally, TPVA material retains excellent hydration after 120 h, demonstrating a significant enhancement in water retention. TPVA-based ZABs achieved a power density of 46.1 mW cm −3 , which is 3.1 times enhancement than that of PVA-based (14.9 mW cm −3 ), and demonstrated significantly extended cycling stability, maintaining stable charge–discharge operation for 35.7 h, outperforming PVA system (11.5 h). Dynamic simulation revealed TEA-PVA interactions, with TPVA showing denser hydrogen bond networks and lower potential energy. This work proposes a promising approach to enhance PVA hydrogel electrolytes for flexible ZABs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2025
·
IF 12.1
Wenyu Zhang,Nan Zhang,Wenhui Zhu,Ling Zhao,Yansheng Gong,Jun Jin,Rui Wang,Huanwen Wang,Beibei He
Zinc-air batteries (ZABs) are highly promising for flexible electronics due to their high energy density and cost-effective. However, their practical application is impeded by the sluggish kinetics of the oxygen evolution and oxygen reduction reactions (OER/ORR). This study presents a novel design featuring BaO nanoparticles anchored on layered perovskite PrBaMn 1.5 Co 0.5 O 6-δ (PBMC) nanofibers, fabricated through a plasma method. Notably, the plasma treatment induces the selective exsolution of A-site Ba onto the perovskite surface, while simultaneously driving the transformation of PBMC from a simple perovskite to a layered perovskite, resulting in a unique BaO/PBMC heterostructure. Theoretical calculations demonstrate that the construction of the BaO/PBMC heterojunction regulates interfacial electronic redistribution, thereby lowering energy barriers for both OER and ORR. Consequently, the BaO/PBMC air electrode exhibits superior peak power density and enhanced stability in flexible solid-state ZABs, compared to the pristine PBMC cathode. Selective A-site exsolution coupled with phase transition, featuring a unique alkaline-earth metal oxide/perovskite heterostructure, may offer new insights for energy conversion technologies.
研究领域:
材料科学
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能源技术
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Energy & Environmental Materials
·
2021
·Vol. 5
·期 2
·543-554
·
IF 15.122
Yu Ma,Ding Chen,Weijun Li,Yapeng Zheng,Lin Wang,Gang Shao,Qiao Liu,Weiyou Yang
The design of efficient cathode with great cycle performance, high flexibility, and low cost is essential for the commercialization of zinc–air battery (ZAB). Herein, we report the exploration of freestanding bifunctional cathode with rationally designed structures, namely, tiny Co nanoparticles embedded in N-doped carbon nanofiber aerogels, which have desired features including uniform Co dispersity, balanced distribution of N-C species, hierarchically porous structure with increased fraction of meso- to micropores, and moderate amounts of defects. Accordingly, the as-fabricated cathodes exhibit positive half-wave potential of 0.82 V for oxygen reduction and small overpotential of 350 mV at 10 mA cm −2 for oxygen evolution, respectively, which deliver smaller reversible oxygen electrode index (0.76 V) than the commercial Pt/C+RuO 2 (0.80 V) and most Co-based electrocatalysts ever reported. Impressively, the as-constructed liquid rechargeable ZAB behaves high peak power density (160 mW cm −2 ), large specific capacity (759.7 mAh g −1 at 10 mA cm −2 , tested after 120 h of OCV tests), and robust stability over 277 h. Moreover, the as-assembled quasi-solid-state ZAB using such freestanding cathode represents excellent mechanical flexibility and outstanding cycle performance, regardless of being serviced under extremely bending conditions from 0° to 180°, underscoring their promising applications as durable bifunctional cathode for portable metal–air batteries.
研究领域:
材料科学
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能源科学
✓ 已验证
DOI
高影响因子
Materials Today Energy
·
2021
·
IF 7.311
Ruopeng Li,Qingyang Li,Lihui Xiao,Xinxin Bai,Shanshan Ji,Jinqiu Zhang,Maozhong An,Peixia Yang
Zinc–air batteries are regarded as ideal candidates for next-generation energy conversion and storage devices, but their conversion efficiency is mainly limited by the sluggish kinetics of the oxygen evolution reaction (OER). Therefore, development of highly active and durable non-noble-metal OER catalysts is of great significance to promote their industrialization process. Herein, we electrodeposit amorphous CoSe 2 ultrathin nanosheet arrays which exhibit a low overpotential of ∼0.287 V at 10 mA/cm 2 and a Tafel slope of ∼62 mV/dec toward the OER in 1 M KOH. This catalytic activity is superior to their crystalline counterpart, commercial RuO 2 , and most of the reported Co-based catalysts. It can be mainly attributed to the lowered adsorption free energy of OER intermediates and improved charge transfer ability with a phase transformation from the crystalline state to the amorphous state, besides the intrinsic catalytic activity of CoSe 2 . When serving as an air cathode in a zinc–air battery, the amorphous CoSe 2 also realizes a larger power density and a better long-term cyclability compared with those of crystalline CoSe 2 and Pt/C–RuO 2 electrodes. This work offers a new underpotential deposition strategy to fabricate high-activity amorphous catalysts and demonstrates its great potential for practical applications.
研究领域:
材料科学
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电化学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·
IF 27.4
Leilei Yin,Mingzi Sun,Shuai Zhang,Yongkang Huang,Bolong Huang,Yaping Du
Currently, there are still obstacles to rationally designing the ligand fields to activate rare-earth (RE) elements with satisfactory intrinsic electrocatalytic reactivity. Herein, axial coordination strategies and nanostructure design are applied for the construction of La single atoms (La-Cl SAs/NHPC) with satisfactory oxygen reduction reaction (ORR) activity. The nontrivial LaN 4 Cl 2 motifs configuration and the hierarchical porous carbon substrate that facilitates maximized metal atom utilization ensure high half-wave potential (0.91 V) and significant robustness in alkaline media. The aqueous and flexible Zinc-air battery (ZAB) integrating La-Cl SAs/NHPC as the cathode catalyst exhibits a maximum power density of 260.7 and 68.5 mW cm −2 , representing one of the most impressive RE-based ORR electrocatalysts to date. Theoretical calculations have demonstrated that the Cl coordination evidently modulate the electronic structures of La sites, which promoted electron transfer efficiency by d-p orbital couplings. With enhanced electroactivity of La sites, the adsorptions of key intermediates are optimized to alleviate the energy barriers of the potential-determining step. Importantly, this preparation strategy is also successfully applied to other REs. This work provides perspectives for near-range electronic structure modulation of RE-SAs based on a nonplanar coordination micro-environment for efficient electrocatalysis.
研究领域:
材料科学
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电化学
·
理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Tiantian Fu,Lingtao Sun,Guijun Li,Yang Xiang,Yibo Tang,Jingqi Sha,Ying Lei,Zhongping Xiong,Yujun Si,Chaozhong Guo
A nitrogen and sulfur codoped carbon-based catalyst (Fe-NS-AG-C) to oxygen reduction reaction (ORR) is prepared by pyrolyzing a precursor from iron chloride, thiourea, anhydrous glucose and carbon black. Glucose is transformed to carbon sheets with defect-rich structures which are highly active to the anchoring of nitrogen and sulfur atoms. Correspondingly, the 3.35 at% and 0.63 at% contents of nitrogen and sulfur in Fe-NS-AG-C are heavily higher than the 0.71 at% and 0.26 at% in the controlled catalyst Fe-NS-C (without glucose). The edge-oriented pyridinic N is easily formed as ORR active sites with the C-S structure. A dual mesopore-dominated microstructure is also constructed by the carbon sheets to favor the mass transfer in the reaction process. As a result, the Fe-NS-AG-C presents outstanding ORR performance with more positive half wave potential, greater limiting current density, and better methanol tolerance than the benchmark Pt/C catalyst. The Zn-air battery assembled with Fe-NS-AG-C outputs 1.48 V of open circuit voltage, 156 mW cm −2 of maximum power density, and 1.26 V of work voltage, 785 mAh g −1 Zn of specific capacity and 983 mWh g −1 Zn of specific energy density at 10 mA cm −2 of discharge current density.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Kexin Huang,Zhongyun Yang,Ling Liu,Xue Yang,Youjun Fan,Miaolan Sun,Chengzhou Liu,Wei Chen,Jun Yang
We herein propose a dual ligand coordination strategy for deriving puissant non-noble metal electrocatalysts to substitute valuable platinum (Pt)-based materials toward oxygen reduction reaction (ORR), a key reaction in metal-air batteries and fuel cells. In brief, cobalt ions are firstly double-coordinated with proportionate 2-methylimidazole (2-MeIm) and benzimidazole (BIm) to obtain drum-like zeolitic imidazolate frameworks (D-ZIFs), which are then carbonized to output the final Co, N co-doped porous carbon (Co–N–PC D ) catalyst inheriting the drum-like morphology of D-ZIFs. The Co–N–PC D is featured by mesopores and exhibits superb electrocatalytic behavior for ORR. Impressively, the half-wave potential of Co–N–PC D catalysts is 0.886 V with finer methanol-tolerance and stability than those of commercial Pt/C. Additionally, a zinc-air battery assembled from the Co–N–PC D displays an open-circuit voltage of 1.413 V, comparable to that of commercial Pt/C (1.455 V), suggesting the potentials of Co–N–PC D in practical energy conversion devices.
研究领域:
材料科学
·
电化学
·
能源转换
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Xiaojie Tan,Fengliang Cao,Xuan Han,Libo Wang,Zhengqiu He,Jinqiang Zhang,Yikun Zhao,Wei Deng,Hui Ning,Zhongtao Li,Qingshan Zhao,Mingbo Wu
Iron-nitrogen-carbon (Fe-N-C) single-atom materials have emerged as the most promising catalysts for the oxygen reduction reaction (ORR), which yet suffers from inadequate stability arising from the attack of ·OH and HO 2 · radicals generated by H 2 O 2 . In this study, density functional theory (DFT) calculations reveal that the presence of peripheral S atoms can regulate the electronic structure of the Fe center and suppress the formation of H 2 O 2 to enhance the catalyst's durability. Thereafter, atomic Fe-N 4 with peripheral S doping is intricately engineered in defect-rich porous carbon nanoshells (Fe-NS-C) through an adsorption-pyrolysis method. The incorporation of S not only optimizes the coordination microenvironment of Fe-N 4 but also induces a larger specific surface area and richer defects. The Fe-NS-C catalyst displays remarkable ORR performance, featuring a half-wave potential (E 1/2 ) of 0.90 V. Its low H 2 O 2 yield (below 1.1 %) and excellent stability (10 mV day in E 1/2 after 10,000 cycles) further underscore the superiority of Fe-NS-C. When employed as the cathode for Zn-air battery, Fe-NS-C achieves an impressive peak power density of 230.1 mW cm −2 and stable charge/discharge potentials over an extended duration of 150 h. This study presents an effective strategy for engineering efficient and durable single-atom electrocatalysts for ORR and Zn-air batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Shuyan Lin,Yongxiang Wang,Xinyu Jing,Haonan Shen,Yide Hao,Zongyu Zhang,Jiangshan Gao,Yan He
The agglomeration phenomenon of metals in transition metal-based carbon catalysts has been one of the major reasons hindering their replacement of commercial Pt/C. Its self-aggregation phenomenon greatly limits the number of active sites and reactivity, which affects the catalytic performance. To overcome this issue, this work prepared a high N-doped carbon structure catalyst coated with high-dispersion FeCo/Fe 3 C nanoparticles. This was achieved by utilizing the advantages of the Prussian blue analogs (PBA) metal framework structure to suppress the self-aggregation of metals, thereby achieving high dispersion. Additionally, the introduction of melamine compensated for the nitrogen loss caused by the carbonization of PBA, thus increasing the nitrogen doping content. The experimental results show that when the calcination temperature is 850 °C and the mass ratio of melamine to FeCo PBA is 5, the half-wave potential (E 1/2 ) of the FeCo@NC catalyst prepared can reach 0.857 V, and the current intensity of FeCo@NC catalyst can maintain 97.12 % during 40,000 s stability test, which is much higher than that of commercial Pt/C. Moreover, the prepared FeCoNC@-850-5 and commercial Pt/C catalysts were used as cathode catalysts for Zn-air batteries (ZAB), and FeCoNC@-850-5 had higher open-circuit voltage (OCV), power density, and specific capacity. These findings demonstrate that the catalyst possesses excellent catalytic activity and promising application prospects, providing a new perspective for the design of efficient oxygen reduction catalysts based on the coupling of bimetallic alloys and N-doped carbon materials.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）