Frontiers in Chemistry
·
2018
·
IF 4.155
Song Xing,Luo Shuiping,Fan Xiaokun,Tang Min,Zhao Xixia,Chen Wen,Yang Qi,Quan Zewei
Well-defined PtNi nanocrystals represent one of the most efficient electrocatalysts to boost the oxygen reduction reaction (ORR), especially in the shape of octahedrons, nanoframes, and nanowires. However, the synthesis of complex PtNi nanostructure is still a great challenge. Herein, we report a new class of PtNi hexapods with high activity and stability toward ORR. The hexapods are prepared by selective capping and simultaneous corrosion. By controlling the oxidative etching, PtNi polyhedrons and nanoparticles are obtained, respectively. The intriguing hexapods are composed of six nanopods with an average length of 12.5 nm. Due to their sharp tips and three-dimensional (3D) accessible surfaces, the PtNi hexapods show a high mass activity of 0.85 A mgPt-1 at 0.9 V vs. RHE, which are 5.4-fold higher than commercial Pt/C, also outperforming PtNi polyhedrons and PtNi nanoparticles. In addition, the mass activity of PtNi hexapods maintains 92.3% even after 10,000 potential cycles.
研究领域:
材料科学
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电化学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Rui Wang,Hongcen Yang,Niandi Lu,Shulai Lei,Dali Jia,Zhixia Wang,Zhenhua Liu,Xiaogang Wu,Hanzhen Zheng,Salamat Ali,Fei Ma,Shanglong Peng
Developing highly active and robust non-noble metal bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of dominant significance for global applications in rechargeable Metal-air Batteries. Fine-tuning the exposed active sites is a competent way to improve their performance. Herein, the NaCl template-assisted strategy for rationally designing a three-dimensional cellular structured nitrogen-doped carbon matrix integrated with nano-scaled Co species has been developed. The resulting electrocatalyst (3D Co/N-C) exhibits a positive half-wave potential of 0.84 V (vs RHE) in ORR, and a low potential of 1.56 V (vs RHE) at 10 mA cm −2 during OER process. Moreover, 3D Co/N-C based Zn-air Batteries (ZABs) exhibit excellent battery performance, especially remarkable power density. The poisoning experiments and DFT calculations identify active sites as pyridinic N and Co during ORR and OER processes, respectively. This work provides a general and easy-to-perform tactic to design bifunctional catalysts, thus helps precisely modulate effective components for ZABs.
研究领域:
电化学
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材料科学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 16
·160536
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IF 3.721
Yizhao Tang,Hao Cheng,Qinggang He,Hanyu Li,Yue An,Jian Xie,Ronghai Liu
Through a facile, stepwise approach that includes electropolymerization, calcination, a hydrothermal method and low-temperature adsorption, a carbon array was coated with RuO2/MnO2 to form a highly efficient composite catalyst (RuO2/MnO2@carbon array) for Li–O2 batteries. The unique, hierarchical, three-dimensional array-type structure facilitates electrode wetting and oxygen transport as well as providing a large volume for Li2O2 loading. The growth of MnO2 nanosheets on the carbon array surface alters the surface roughness and provides attachment sites for the subsequent loading of catalyst nanoparticles. In addition, the introduction of RuO2 induces the formation of Mn3+ on the surface of MnO2, which not only improves the electrode conductivity but also the catalytic activity for ORR/OER. As a result, conformal growth of thin layers of Li2O2 on the surface of the RuO2/MnO2@carbon array and reversible decomposition of Li2O2 during cycling were achieved. In comparison with cathodes without a carbon array or catalyst, the Li–O2 cell with a RuO2/MnO2@carbon array cathode exhibits an markedly improved performance with high discharge capacity (10 000 mAh g−1 at 100 mA g−1) and long cycling life (252 cycles at 200 mA g−1 with a limited capacity of 500 mAh g−1).
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2024
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IF 5.2
Siyuan Wang,Yunze Zhang,Jian Wang
Rationally designing highly active electrocatalysts for the oxygen reduction reaction (ORR) without relying on precious metals is critical for promoting the application of metal–air batteries and fuel cells. As a promising alternative to traditional Pt-group-based catalysts, transition-metal oxides (TMOs) with high corrosion resistivity and diverse structure configuration have exhibited great catalytic potential. However, the current favorable ORR performance of TMOs has often been achieved through their coupling with engineered carbons such as graphene and carbon nanotubes, which can obscure the intrinsic catalytic potential of TMOs. To promote TMO-based catalysts for ORR applications, comprehensively analyzing their catalytic properties and screening promising TMO-based parent materials is crucial. Herein to eliminate the research gap, 22 noble-metal-free TMOs (e.g., Co3O4, MnO, and Fe2O3) were benchmarked for ORR catalysis, with Pt/C and RuO2 as comparisons. Nb2O5 demonstrated the greatest potential as an ORR electrocatalyst among all of the studied TMOs, with higher specific activity surpassing that of Pt/C. In addition, it could achieve a larger peak power density than Pt/C in a more practical Zn–air battery setup, showing promise for applications. Regarding stability, most of the studied TMOs exhibited larger losses in limiting current densities than the degradation of half-wave potentials (from 0.65% to 7.54) after the 10,000 cycle accelerated degradation tests, pointing out the direction to improve their ORR stabilities.
研究领域:
电化学
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材料科学
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能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 10
·4823-4832
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IF 3.5
Haihui Hu,Ke Ma,Yuandong Yang,Na Jin,Linjie Zhang,Jinjie Qian,Lili Han
Hydrogen peroxide (H2O2) electrosynthesis via the two-electron oxygen reduction reaction (2e− ORR) represents a green alternative to the energy-intensive anthraquinone process. However, the practical application of this method is limited by the lack of cost-effective and high-performance electrocatalysts. Reported here is a hybrid catalyst composed of nickel (Ni) clusters immobilized onto the surface of two-dimensional siloxene nanosheets (Ni/siloxene), which exhibits excellent efficiency and selectivity in electrocatalytic oxygen reduction to H2O2 in an alkaline medium, demonstrating a standard 2e− pathway with >95% H2O2 selectivity across a wide potential range. Experimental results disclose that the high performance of Ni/siloxene can be traced to a synergy of the Ni clusters and the oxygen-rich surface of siloxene. Density functional theory (DFT) calculations further reveal a weakened interaction between Ni/siloxene and *OOH and the consequently reduced energy barrier for the *OOH protonation toward H2O2 desorption, thus leading to a high 2e− ORR reactivity and selectivity. This work provides a valuable and practical guidance for designing high-performance 2e− ORR electrocatalysts based on the rational engineering of the metal–support interaction.
研究领域:
材料科学
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电化学
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催化
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Chencheng Dong,Zhi-Qiang Wang,Chao Yang,Xiaomeng Hu,Pei Wang,Xue-Qing Gong,Lin Lin,Xiao-yan Li
Oxygen reduction reaction (ORR) can realize the goal of in-situ H 2 O 2 generation. A suitable catalyst ensures a proper binding strength between the electrocatalyst and the intermediate (i.e., *OOH), thereby avoiding the 4-electron ORR process and H 2 O production. Herein, we demonstrate that single molybdenum (Mo) atoms/clusters doped on carbon nanotubes can effectively alter the ORR pathway to generate H 2 O 2 ; meanwhile, the established sequential ORR system for H 2 O 2 production can tandemly remove ibuprofen (IBU) and other organic contaminants from water and wastewater. The results reveal that single atomic Mo clusters preferentially acted as the active sites that are merely required to overcome 0.11 eV downhill to form *OOH. Surprisingly, this tandemly constructed ORR with in-situ generated H 2 O 2 performed better than the in-vitro H 2 O 2 system. These findings offer a promising solution to reduce the costs related to the production and transportation of H 2 O 2 for various applications, including the oxidation and removal of emerging organic contaminants from water and wastewater.
研究领域:
环境科学
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催化
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水处理
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Kuang Sheng,Qingfeng Yi,A-Ling Chen,Yuebing Wang,Yuhui Yan,Huidong Nie,Xiulin Zhou
Searching for high-quality air electrode catalysts is the long-term goal for the practical application of Zn–air batteries. Here, a series of coexistent composite materials (CoNi/NHCS-TUC-x) of cobalt–nickel supported on nitrogen-doped hollow spherical carbon and tubular carbon are obtained using a simple pyrolysis strategy. Co and Ni in the composites are mainly present in the form of alloy nanoparticles, M–Nx and M–Cx (M = Co or Ni) species, with high oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) electroactivity. The materials containing different proportions of spherical carbon and tubular carbon obtained by simply adjusting the raw materials for generating tubular carbon exhibit interesting bifunctional performance: samples with an abundant tubular content have the highest ORR onset potential (0.91 V vs reversible hydrogen electrode), while those with a rich spherical content have the highest ORR current density (5.13 mA·cm–2). Furthermore, CoNi/NHCS-TUC-3 provides the lowest potential difference (ΔE = Ej=10 – E1/2) of 0.806 V. We then test the potential possibility of CoNi/NHCS-TUC-3 as an air electrode for primary and rechargeable Zn–air batteries. The primary battery delivers an open-circuit potential of 1.59 V, a peak power density of 361.8 mA·cm–2, and a specific capacity of 756.5 mA h·gZn–1. The rechargeable battery could be cycled stably for more than 55 h at 10 mA·cm–2. These characteristics make CoNi/NHCS-TUC-3 a superior electrocatalyst for both the ORR and OER, as well as a suitable bifunctional electrode applied to a rechargeable Zn–air battery.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Nanoscale
·
2022
·Vol. 14
·期 48
·17995-18002
·
IF 8.307
Lian-Hua Xu,Wen-Ju Wang,Xue-Ji Zhang,Serge Cosnier,Robert S. Marks,Dan Shan
Due to the complexity of the synthetic process of cobalt phosphides (CoP), ongoing efforts concentrate on simplifying the preparation process of CoP. In this work, amino tris(methylene phosphonic acid) (ATMP, L1) and melamine (MA, L2) are assembled into two-dimensional (2D) organic nanostructures by hydrogen bonding and ionic interactions via a supramolecular assembly, which greatly weakens the coordination ability of L1 with Co2+. As the introduced L2 is rich in carbon and nitrogen, it allows the cobalt–organophosphate complex to be placed under a strongly reducing atmosphere during the high-temperature calcination process to achieve an in situ phosphating purpose. The resulting catalyst (N-CoP/NC) exhibits the sought-after enhanced oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) performance. For the ORR in 0.1 M KOH, an enhanced onset potential (0.908 V vs. RHE) and diffusion limiting current (6.280 mA cm−2) can be obtained, which is comparable to those of 20% Pt/C (0.911 V vs. RHE, 5.380 mA cm−2). For the HER in 0.5 M H2SO4, an overpotential of 150 mV is required to drive a current of 10 mA cm−2. Moreover, Density Functional Theory (DFT) calculations reveal the catalytic pathway of N-CoP/NC.
研究领域:
材料科学
·
电催化
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·Vol. 49
·期 14
·5981-5988
·
IF 2.5
Wenting Liu,Feng Wang,Xiaoyu Wu,Zhenzhen Wu
Non-precious metal catalysts have been extensively developed for metal–air batteries and fuel cells with the aim of reducing economic costs in practical applications. This paper reports a strategy involving the loading of biomass-derived nitrogen-doped porous carbon materials with NiCo alloy nanoparticles to fabricate high-performance bifunctional catalysts towards oxygen reduction and evolution reactions. The resulting catalyst demonstrates considerable catalytic activity with exceptional long-term cycling stability and methanol resistance. This material offers a reference strategy for the economical and environmentally sustainable large-scale manufacturing of renewable bifunctional catalysts.
研究领域:
材料科学
·
催化化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Mingyang Liu,Qi Li,Xudong Xiao,Xuena Ma,Xiaoqin Xu,Yihang Yin,Bin Zhang,Minghui Ding,Jinlong Zou,Baojiang Jiang
Interface engineering has been recognized as one of the most promising strategies for tuning the catalytic properties of catalysts. However, building well-defined nanointerfaces for efficient oxygen reduction/evolution reactions (ORR/OER) remains a challenge. Herein, a hollow heterostructure composed of highly-dispersed CoTe 2 inside the mesoporous walls of nitrogen-doped carbon nanoboxes and uniformly-dispersed NiTe 2 outside the mesoporous walls (H-CoTe 2 /NiTe 2 @NCBs) is designed via a ZIF67-involved etching-anchoring-tellurization strategy. Promising half-wave potential of 0.86 V and overpotential of 320 mV at 10 mA cm −2 are obtained by H-CoTe 2 /NiTe 2 @NCBs. The excellent ORR/OER activity of H-CoTe 2 /NiTe 2 @NCBs is ascribed to the synergistic coupling based on nanointerfaces between CoTe 2 and NiTe 2 . Density functional theory calculations confirm that the nanointerface-based electronic coupling between CoTe 2 and NiTe 2 facilitates the charge transfer between two components and generates abundant catalytically active sites at the heterointerface, thereby significantly promoting the ORR/OER activities. This work provides the design principles for transitional bimetallic tellurides as bifunctional electrocatalysts.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2024
·Vol. 171
·期 6
·066502
·
IF 3.1
Guang Li,Xiangmei Tang,Kuang Sheng,Can Fang,Yiduo Zeng,Zhaomin Lu,Yaping Wang,Hu Zhou,Qingfeng Yi
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.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xue Liu,Wei Yan,Jie Song,Hao Song,Wenmiao Chen,Yuexing Zhang,Yanli Chen
Enhancing the exposure of active sites and optimizing the electronic structure of the catalysts are indispensable for efficient catalyst design, yet remains challenging in the renewable energy field. Herein, a sequential pyrolyzing and phosphating approach for a well-designed GO/CoTPP gel precursor has been explored to prepare a Co-based carbon catalyst containing single-atom Co-N x and hollow Co 2 P active species (Co 2 P/Co-N-C) for multifunctional electrocatalytic reactions. Kirkendall effect occurring during the template-free one-pot phosphating approach induced the formation of the hollow Co 2 P structure in the catalyst, simultaneously optimizing the electron structure and allowing the active sites to be exposed to a greater extent. DFT calculations demonstrated that the Co 2 P and Co-N x structures enable Co 2 P/Co-N-C to have a suitable d-band center depending on the electron transfer from Co 2 P to Co-N x , which enhances the adsorption of O* and the dissociation of OH* in oxygen electrode reactions, thereby facilitates catalytic reactions. As a result, the Co 2 P/Co-N-C exhibits excellent trifunctional activity with a half-wave potential of 0.89 V in alkaline for oxygen reduction reaction (ORR), overpotentials of 330 mV for oxygen evolution reaction (OER) and 190 mV for hydrogen evolution reaction (HER), respectively, which are among the best results reported to date for Co-containing carbon-based catalysts. Furthermore, the flexible Zinc-air battery with Co 2 P/Co-N-C electrodes also demonstrates a high open circuit voltage of 1.35 V, which is applied to build the self-powered device for water splitting continuously. Our work provides a facile strategy to prepare high-performance trifunctional catalysts by morphology/structure control of metal-based NPs on carbon-based materials.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 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）