ACS Applied Nano Materials
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2024
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IF 5.3
Minghao Dou,Wensong Wang,Xiang Liu,Mengjie Yao,Kai Ding,Weiwei Lin,Xiuwen Cao,Chaoyue Li,Shenjie Li,Yanyan Chen
Compared with the oxygen precipitation reaction (OER), the theoretical application of urea oxidation reaction (UOR) with a smaller potential is more conducive to achieve H2 release, showing a strong application prospect in the field of wastewater treatment. However, the efficiency of the traditional nickel foam-based catalyst is still subject to the following two factors: the high oxidation potential of Ni3+ and the uncertainty of the oxidation and reduction active sites. Here, with the advantage of two-dimensional sheet porous high surface area, a Ni(OH)2 nanosheet was prepared by depositing ZIF-67 to inhibit the formation of Ni3+ and maximize the space utilization. Then, the NiS/Co3S4/Ni3S2 nano heterostructure was constructed to improve the interface electronic structure and optimize the adsorption energy of the intermediates via in situ vulcanization. The NiS shell on the surface of the catalyst provides sufficient reaction sites for the catalytically active substance NiOOH generated during the UOR at a lower oxidation potential. At a current density of 50/100 mA cm–2, the overpotential is only 1.330/1.340 V while maintaining the catalytic durability for 20 h. At the same time, the NiS/Co3S4/Ni3S2/NF nano heterostructure material shows good urea degradation performance and stability, which provides the possibility of degradation and treatment of industrial, agricultural, and domestic wastewater containing urea.
研究领域:
材料科学
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环境科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2025
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IF 3.9
Yongxuan Xiang,Wenji Li,Jiapeng Wang,Hongyue Tong,Xinmiao Li,Hua-Bin Yuan,Ziwei Wu,Guoqiang Chen,Tieling Xing
Metal–organic framework (MOF) materials have been extensively utilized in water electrolysis owing to their versatile chemical configurations and three-dimensional porous and exceptional surface areas characteristics. This study implemented an MOF-derived synthesis approach to develop a self-supporting electrocatalytic system. Initially depositing nanostructures on flexible carbon cloth through controlled growth, subsequent thermal treatment, and solution-phase sulfurization processes generated the Co3S4/Ni3S2@CC composite. The engineered material demonstrates hierarchical porosity and synergistic interfacial effects between components, facilitating numerous catalytic centers and optimized electron transport pathways. Strategic sulfur incorporation successfully tailors the electronic environment, substantially boosting the reaction kinetics. The integrated heterointerface electrode manifests superior dual-functional performance in alkaline freshwater electrolysis, demonstrating remarkably low overpotentials of 169 mV (HER) and 294 mV (OER), respectively, to attain a 10 mA cm–2 current density, while maintaining excellent durability under continuous operation. When operating in saline environments, the catalyst demonstrates remarkable catalytic activity, exhibiting overpotentials of 177 mV for the HER and 323 mV for the OER under identical current density conditions. Introducing ethanol or methanol into the electrolyte system significantly reduces the activation potential and lowers the overall energy requirements. These findings provide crucial guidance for developing advanced MOF-derived transition metal electrocatalysts optimized for efficient water splitting applications.
研究领域:
电化学
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能源转换与存储
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纳米材料
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催化
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可再生能源
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Qi Xue,Pengjing Yin,Runmiao Chen,Juan Bai,Haoqi Yang,Yuanzhen Zhou
A self-supported Mo-doped Co 3 S 4 /Ni 3 S 2 heterostructure was constructed. • HER and OER overpotentials reach 45.6 and 51.5 mV at 10 mA cm −2 . • Operando Raman reveals earlier formation of a NiOOH-dominated active phase. • Mo suppresses excess OH ⁎ coverage and accelerates oxygen-intermediate turnover. • A symmetric electrolyzer delivers 10 mA cm −2 at a cell voltage of 1.43 V. Dynamic reconstruction of transition-metal sulfides into active oxyhydroxides is critical to the oxygen evolution reaction (OER), yet promoting this transformation at a low anodic potential while avoiding excessive accumulation of oxygenated intermediates remains challenging. Herein, density functional theory (DFT) calculations were used to reveal the electronic effect of Mo incorporation on the Co 3 S 4 /Ni 3 S 2 heterointerface, showing a downward shift of the Ni d -band center and reduced electron localization around adjacent Ni and Co sites. Based on this insight, a self-supported Mo-doped Co 3 S 4 /Ni 3 S 2 heterostructure was synthesized on nickel foam (Mo-Co 3 S 4 /Ni 3 S 2 ). The optimized Mo 0.03 -Co 3 S 4 /Ni 3 S 2 requires overpotentials of only 51.5 mV and 45.6 mV to deliver 10 mA cm −2 for OER and HER. A two-electrode electrolyzer using Mo-Co 3 S 4 /Ni 3 S 2 as both electrodes reaches 10 mA cm −2 at only 1.43 V. Methanol-probe measurements indicate reduced OH ⁎ accumulation after Mo incorporation, while in-situ Raman spectroscopy identifies the reconstructed NiOOH layer as the OER-active phase and reveals its formation at a lower anodic potential. Further calculations show that Mo brings hydrogen adsorption closer to thermoneutral and lowers the thermodynamic limitation of OER by regulating oxygenated-intermediate adsorption. This work provides a general strategy for regulating dynamic catalyst reconstruction and interfacial reaction processes, which may advance the development of efficient electrocatalysts for sustainable hydrogen production. Download: Download high-res image (132KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Xuanning Qin,Han pang,Zebin Yu,Zuoyu Qin,Ronghua Jiang,Shuangquan Yao,Jun Huang,Yanping Hou,Ben Fan
Accelerating electron transfer and exposing active sites are key factors that could improve electrocatalytic hydrogen evolution reaction (HER). In this study, Co 3 S 4 -Ni 3 S 2 -C/N, the cactus bulb-shaped nanoparticles based on metal-organic frameworks (MOFs), were successfully prepared. The catalyst requires only 101 and 227 mV overpotential to reach current densities of 20 and 100 mA cm −2 , respectively, in 1 M KOH. The high catalytic activity is attributed to the confinement effect achieved by introducing 2-aminoterephthalic acid as a precursor, allowing the catalyst to have a small particle size and fully exposed metal active sites. Moreover, the catalyst has a highly conductive metal-S-C/N channel that effectively reduces the intrinsic charge transfer resistance of the catalytic electrode, improves its conductivity, and modulates the electron density at the metal active site. Furthermore, compared to other crystal planes, the exposed (111) crystal plane of Co 3 S 4 provides the most octahedral coordination of high spin state Co 3+ , which is highly catalytically active. This makes it the dominant crystal plane for catalysis. Through spatial confinement effect to limit metal sulfide particle size and introducing an organic backbone to create highly conductive metal-S-C/N channels, our study provides a general approach to developing highly active catalytic materials.
研究领域:
材料科学
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电化学
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纳米技术
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催化
✓ 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）