Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Zhang Zhen,Xing Zhenyu,Luo Xianglin,Cheng Chong,Liu Xikui
Dual-atom catalysts featuring synergetic dinuclear active sites, have the potential of breaking the linear scaling relationship of the well-established single-atom catalysts for oxygen reduction reaction; however, the design of dual-atom catalysts with rationalized local microenvironment for high activity and selectivity remains a great challenge. Here we design a bisalphen ladder polymer with well-defined densely populated binuclear cobalt sites on Ketjenblack substrates. The strong electron coupling effect between the fully-conjugated ladder structure and carbon substrates enhances the electron transfer between the cobalt center and oxygen intermediates, inducing the low-to-high spin transition for the 3 d electron of Co(II). In situ techniques and theoretical calculations reveal the dynamic evolution of Co 2 N 4 O 2 active sites and reaction intermediates. In alkaline conditions, the catalyst exhibits impressive oxygen reduction reaction activity featuring an onset potential of 1.10 V and a half-wave potential of 1.00 V, insignificant decay after 30,000 cycles, pushing the overpotential boundaries of ORR electrocatalysis to a low level. This work provides a platform for designing efficient dual-atom catalysts with well-defined coordination and electronic structures in energy conversion technologies.
研究领域:
材料科学
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催化化学
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能源转换技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 31
·19968-19978
·
IF 10.7
Zicheng Huang,Wenjie Shao,Yijuan Zheng,Junyu Wang,Mao Wang,Shuang Li,Xiaohui Xu,Chong Cheng,Changsheng Zhao
Transition metal oxide-based catalysts are known as the most active oxygen evolution reaction (OER) catalysts due to their intrinsic electronic structures and binding strength of oxygenated intermediates. However, even the most active transition metal oxide-based OER catalysts have a turnover frequency far lower than that of the oxygen-evolving complexes in biological systems for intermolecular site aggregation. Herein, we implement the hybridization of a metal–organic framework and tungstic acid (WO3·xH2O-in-MIL-88) to achieve ordered FeNi site isolation at the molecular level and avoid intermolecular decomposition during the catalysis process. The optimized hybrid with 15% tungstic acid (15%-WO3·xH2O-in-MIL-88) achieves a much-enhanced OER activity and stability in terms of a low overpotential of 263 mV to reach a current density of 10 mA cm−2, a low Tafel slope of 39 mV dec−1, and long-term stability, which is much superior to that of the commercial RuO2 catalyst.
研究领域:
材料化学
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电化学
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催化化学
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能源科学
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无机化学
✓ 已验证
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Yuyang Xue,Qi Li,Aijuan Xie,Shiping Luo
Water splitting is a key and efficient method for hydrogen production. A major hurdle in overall water decomposition is developing affordable, highly active electrocatalysts to boost hydrogen (HER) and oxygen (OER) evolution reactions. In this work, influence of sulfur/ phosphorus co-doping sequence on the performance of NiFe(OH) x catalyst on the surface of nickel foam (NF) for overall water splitting was investigated. The findings of the experiment indicate that NiFe 0.4 P 1.2 S 1.6 /NF exhibits an overpotential of 67 mV for HER and 106 mV for OER at 10 mA cm −2 . Additionally, the Tafel slopes are reported as 60.92 mV dec -1 and 18.87 mV dec -1 , correspondingly. Electrochemical impedance spectroscopy reveals that NiFe 0.4 P 1.2 S 1.6 /NF exhibits low R ct values: 0.88 Ω for HER and 2.58 Ω for OER. Furthermore, its electrochemical active surface areas measure 303.8 cm 2 (HER) and 121.25 cm 2 (OER). Stability and i-t curve tests confirm the robustness of NiFe 0 . 4 P 1 . 2 S 1 . 6 /NF in HER (86.43 % retention) and OER (75.07 % retention) over 10-hour durability tests, maintaining ∼ 87.11 % initial cell voltage. This sulfur-phosphorus codoping method presents a new strategy for efficient HER/OER electrocatalysts.
研究领域:
电催化
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材料化学
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能源科学
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纳米材料
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表面科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materiomics
·
2025
·Vol. 11
·期 6
·101060
·
IF 9.6
Geng Cheng,Wenpei Li,Chengyan Liu,Jie Gao,Jun-Liang Chen,Jianhua Zhou,Xiaoyang Wang,Lei Miao
Two-dimensional (2D) materials such as metal chalcogenides have great potential as cathode catalyst materials for lithium oxygen batteries (LOBs) due to their large specific surface area and stable chemical properties. However, thus far, due to the lack of theoretical prediction methods, huge load on catalytic synthesis and performance evaluation is concerned. Herein, we reported a theoretical method for 2D metal chalcogenides as catalysts for LOBs using first principles density functional theory (DFT) calculations. We extracted key parameters that affect the overpotential, including Li–X bond energy (X represents chalcogen elements) and catalyst lattice constant, and theoretically predicted the catalytic performance. The DFT calculation results indicate that MoS 2 with appropriate Li–X bond energy and lattice constant has the lowest theoretical overpotential, and its cyclic stability should be higher than other materials under the same conditions. Significantly, we experimentally validated the theoretical predictions presented above. The experimental results shows that pure MoS 2 with 2H phase can stably work for more than 220 cycles at a current density of 500 mA/g, and the actual overpotential is lower than other metal chalcogenides. This work provides a swift pathway to accelerate searching high performance catalytic in LOBs.
研究领域:
材料科学
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电化学
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纳米催化
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能源存储
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理论计算化学
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Yaru Huang,Maoting Gan,Shaofeng Ni,Chuan Tan,Xiangwen Gao,Fengjiao Yu
Na O 2 batteries have garnered increasing attention due to their high energy density and the abundance of sodium resources. However, the lack of efficient air cathodes has hindered their practical application, preventing the realization of stable and long cycling lifespans. Herein, we report the Na O 2 batteries using Fe-doped CoP nanowire arrays on carbon cloth (FeCoP-CC) as the air cathode, which exhibit a low overpotential of 200 mV, a high discharge specific capacity of 2853 mAh g −1 , and stable cycling performance over 200 cycles at a current density of 200 mA g −1 . The exceptional electrochemical performance can be attributed to the optimized adsorption of oxygen species by FeCoP-CC, which forms film-like NaO 2 discharge products that facilitate the oxygen transport channels. Furthermore, the film-like discharge products and the extensive contact interface with the cathode accelerate charge transfer and effectively decompose during subsequent charging processes. This work provides valuable insights into the rational design of electrocatalytic air cathodes.
研究领域:
电化学
·
能源材料
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纳米材料
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电催化
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电池技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）