JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Zuohui Wang,Nannan Heng,Xiaobing Wang,Jinling He,Yong Zhao
The original active site units and morphologies structure on catalyst surface is highly important to promote the rate of chemical reaction, while less concern is paid on their dynamic change during reaction process. Understanding these reconstructions in reactions is essential to illustrate the correlations between the structure and reactivity of catalyst, as well as the rational design of efficient catalyst. Here, single metal phophide materials are adopted as model electrocatalysts to show the structure evolution in the process of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). After both OER and HER operation, the core-shell structured metal-hydroxide/oxyhydroxide@metal-phosphide catalysts are generated, resulting in the high but decreased activity. To overcome the activity deterioration of metal phosphide induced by morphology reconstruction, binary heterostructure metal phosphides catalysts are designed and show the better OER and HER activity and stability compared to those of single phosphides. The work illustrates the structure-performance relationship of catalyst surface dynamics on catalytic performance, which will provide the guidance for designing high performance electrocatalysts, photocatalysts, and thermal catalysts.
研究领域:
电化学
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催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Ze-Feng Xu,Chuan-Wu Chen,Ya-Nan Jing,Da-Qiang Liu,Hong-Xin Zhang,Qiu-Xia Lin,Lei-Lei Li,Xing-Liang Yin
Slow kinetics of the oxygen evolution reaction (OER) during water electrolysis limits hydrogen evolution reaction (HER) efficiency. Urea oxidation reaction (UOR), with a lower thermodynamic potential (0.37 V vs. RHE) than OER, offers an energy-saving alternative. Designing robust, multifunctional electrocatalysts for hydrogen generation by water electrolysis remains challenging. In this work, a universal two-stage solvothermal strategy was developed to synthesize α/β-FeOOH-based self-supported hierarchical structure catalysts on arbitrary metal substrates, evading polymeric binders. FeOOH/Fe achieves exceptional HER performance, while FeOOH/Ni delivers superior OER/UOR activity, exhibiting extremely-low UOR kinetics with a 12.24 mV·dec −1 Tafel slope. Asymmetric FeOOH/Ni (+)||FeOOH/Fe (−) electrolyzer requires ultralow voltages of 1.799 V (1.0 M KOH), 1.888 V (seawater/1.0 M KOH), and 1.627 V (0.33 M urea/1.0 M KOH) to drive 300 mA cm −2 , surpassing most similar systems. It maintains >9 Faraday efficiency over 100-h at ≥ 300 mA cm −2 , demonstrating industrial-grade stability. The catalysts’ accessible active sites, accelerated charge transfer, rapid kinetics, and superhydrophilicity synergistically enable rapid mass/electron transport and durable operation. This work provides a scalable platform for binder-free electrocatalysts, advancing practical hydrogen production through urea-assisted electrolysis and seawater utilization.
研究领域:
材料科学
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电化学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Ying Wu,Min Li,Wenhui Fang,Yutao Cao,Shixian Xin,Hong Zhao
Electrochemical water splitting is a promising method for hydrogen production but is restricted by sluggish oxygen evolution reaction (OER), so we propose to replace OER with the thermodynamically preferred glucose oxidation reaction (GOR) to reduce the supply voltage. Herein, hollow RuV-Co(OH) 2 arrays have been fabricated by the hydrothermal method of sacrificing ZIF-67 to codope vanadium (V) and ruthenium (Ru). Electrochemical studies show that RuV-Co(OH) 2 has excellent hydrogen evolution reaction (HER) activity with a low overpotential of 77 mV at the current density of 10 mA cm −2 (η 10 = 77 mV) and good GOR activity. Density functional theory (DFT) calculations indicate that V and Ru tune the electronic structure of RuV-Co(OH) 2 , greatly increasing the density of the active sites. Moreover, RuV-Co(OH) 2 assembled glucose-assisted hydrogen evolution cell exhibits a battery voltage of 1.42 V for a current density of 10 mA cm −2 , a significant reduction of 240 mV compared to overall water splitting along with higher-value glucose oxidation products. Furthermore, RuV-Co(OH) 2 exhibits outstanding stability. Scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) analysis demonstrate that RuV-Co(OH) 2 has superior mechanical stability. This work opens up a new approach to designing novel bifunctional electrocatalysts for energy-saving H 2 production and valuable coproductions.
研究领域:
电化学
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催化
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材料科学
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能源转换与存储
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Zhang Minghao,Sun Chenxi,Chen Guanhong,Kang Yuanhong,Lv Zeheng,Yang Jin,Li Siyang,Lin Pengxiang,Tang Rong,Wen Zhipeng,Li Cheng Chao,Zhao Jinbao,Yang Yang
Rechargeable aqueous zinc-metal batteries, considered as the possible post-lithium-ion battery technology for large-scale energy storage, face severe challenges such as dendrite growth and hydrogen evolution side reaction (HER) on Zn negative electrode. Herein, a three-dimensional Cu-In alloy interface is developed through a facile potential co-replacement route to realize uniform Zn nucleation and HER anticatalytic effect simultaneously. Both theoretical calculations and experimental results demonstrate that this bifunctional Cu-In alloy interface inherits the merits of low Zn-nucleation overpotential and high HER overpotential from individual copper and indium constituents, respectively. Moreover, the dynamical self-reconstruction during cycling leads to an HER-anticatalytic and zincophilic gradient hierarchical structure, enabling highly reversible Zn chemistry with dendrite-free Zn (002) deposition and inhibited HER. Moreover, the improved interface stability featured by negligible pH fluctuations in the diffusion layer and suppressed by-product formation is evidenced by in-situ scanning probe technology, Raman spectroscopy, and electrochemical gas chromatography. Consequently, the lifespan of the CuIn@Zn symmetric cell is extended to more than one year with a voltage hysteresis of 6 mV. Importantly, the CuIn@Zn negative electrode is also successfully coupled with high-loading iodine positive electrode to fabricate Ah-level (1.1 Ah) laminated pouch cell, which exhibits a capacity retention of 67.9% after 1700 cycles.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Qiaohong Zhu,Bocheng Qiu,Huan Duan,Yeteng Gong,Zengwei Qin,Bin Shen,Mingyang Xing,Jinlong Zhang
Bimetallic phosphides have attracted considerable attention in photocatalytic hydrogen evolution reaction (HER), owing to its thermodynamic feasibility. Most reports attributed the HER activity to the reduction of free energy of protonation (ΔG H* ), however, few revealed the whereabouts of the photo-induced electrons, which makes the mechanism of HER not very clear. Herein, nickel-iron bimetallic phosphide (NiFeP) is designed onto graphitic carbon nitride (NiFeP/g-C 3 N 4 ) for the photocatalytic HER, which exhibits a high hydrogen production of 3.549 mmol g −1 h −1 . It is found that the co-catalyst of NiFeP can not only reduce the ΔG H* , but also make the photogenerated electrons transfer directionally, which play a synergistic role in enhancing the activity of HER. The reduction of ΔG H2O and ΔG H* over NiFeP in HER can be well demonstrated by the density functional theory (DFT) calculations. Furthermore, the localized distribution of electrons on the surface of NiFeP is verified by measuring the lifetime of photo-generated carriers combined with the REDOX experiment. The shortened lifetime τ, decreased τ1 and τ2 of NiFeP/g-C 3 N 4 indicate that the photoexcited electrons of g-C 3 N 4 are directly transferred to the co-catalyst surface, contributing to the worse delocalization capacity of electrons on the ca-catalyst and its easier reactions with protons trapped on the co-catalyst surface. Furthermore, the degradation with peroxymonosulfate (PMS) confirms the photogenerated holes over 5NiFeP/g-C 3 N 4 are mainly concentrated on the surface of g-C 3 N 4 to decompose H 2 O for the generation of OH, while the photogenerated electrons are directed to the NiFeP to react with the neighboring PMS or protons to form SO 4 − or H 2 . Besides, the density of state intensity (DOS) also confirms the photogenerated electron migration pathway at the metal-semiconductor (NiFeP-g-C 3 N 4 ) interface. Our research clarifies the mechanism of bimetallic phosphides co-catalytic HER system, which will provide theoretical guidance for the design and preparation of multi-metallic center photocatalytic system with a higher HER activity in the future.
研究领域:
材料科学
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催化
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光化学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 22
·10433-10440
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IF 9.931
Yiping Hu,Feng Li,Yu Long,Haidong Yang,Lili Gao,Xuefeng Long,Haiguo Hu,Na Xu,Jun Jin,Jiantai Ma
Searching for highly efficient, stable and non-noble metal electrocatalysts for the hydrogen/oxygen evolution reaction (HER/OER) is crucial to renewable-energy conversion systems. Cobalt phosphosulfide (CoPS) is regarded as a promising electrocatalyst for the HER in acid solution. Nonetheless, there are no studies of its HER and OER activity in basic solution. Herein, we engineer a novel and highly efficient water splitting electrocatalyst of ultrafine CoPS nanoparticles (NPs) encapsulated in N, P, and S tri-doped porous carbon (CoPS@NPS-C) through metal–organic frameworks (MOFs) and commercial carbon black (XC-72) as precursors. The abundant and evenly distributed metals of MOFs form ultrafine CoPS NPs, and the rich N organic ligands of MOFs and XC-72 are shaped into the NPS-C to protect CoPS NPs leading to long-term stability in water-splitting applications. Meanwhile, the strong interaction between CoPS and NPS-C in this special structure not only ensures the high activity of the HER in acid solution and the OER in alkaline solution, but also maintains good HER performance in alkaline solution. The results display that the novel structure electrocatalyst of CoPS@NPS-C has great potential in water-splitting applications.
研究领域:
材料科学
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电化学
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可再生能源
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催化
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 40
·15536-15545
·
IF 8.262
Zhen Zhu,Yan Yang,Yue Guan,Juanhong Xue,Lili Cui
Hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) are vital in renewable energy technologies, such as water splitting and fuel cells. Nevertheless, increasing efforts have been paid to develop non-precious metal catalysts as alternatives to noble metal catalysts for HER and ORR. However, how to rationally design and construct an advantageous catalyst is still challenging. Here, a novel cobalt-embedded in nitrogen-doped graphene aerogel (Co–N–GA) catalyst is firstly rationally designed and synthesized by employing a facile strategy of implementing the confined growth of metal organic frameworks (MOFs) within graphene aerogels (GAs). It is worth noting that the Co–N–GA exhibits hierarchical porosity involving micropores, mesopores and macropores, as well as a high surface area (466.6 m2 g−1). More importantly, benefiting from the synergetic effect of hierarchical porosity, high surface area, N-doped carbon and the inner Co metal, the catalyst Co–N–GA displays extraordinarily superior activity for both HER at various pH values and ORR along with better stability. Especially for HER, the onset overpotential, overpotentials@10, 100 mA cm−2 and Tafel slope on the catalyst Co–N–GA in 0.5 M H2SO4 are 0 mV, 46 mV, 183 mV and 33 mV dec−1, respectively. Most importantly, these values are much lower than those of almost all prepared noble-metal-free HER catalysts, indicating the excellent activity for HER of our as-prepared catalyst Co–N–GA. Herein, our strategy opens a new platform to construct a variety of hierarchically porous GA-based catalysts that serve as superior electrocatalysts in energy storage and conversion technologies.
研究领域:
材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2024
·
IF 6.1
Liang Mei,Yuefeng Zhang,Zimeng Ye,Ting Han,Honglu Hu,Ruijie Yang,Ting Ying,Weikang Zheng,Ruixin Yan,Yue Zhang,Zhenbin Wang,Zhiyuan Zeng
Fabricating solution-processable composite materials of transition metal dichalcogenides (TMDs) with ultrasmall noble metal structures employing an easy preparation method poses a significant challenge. In this study, we utilized a green, one-step synthetic method by directly employing electrochemical lithium intercalation-based exfoliated metallic TMD nanosheets (MoS2, WS2, and TiS2) to reduce palladium ions (Pd2+) to metallic Pd0, leading to the deposition on their surfaces. The resulting Pd nanoparticles (Pd NPs) in composites (Pd-MoS2, Pd-WS2, and Pd-TiS2) were found to be amorphous, with a size ranging from 0.81 to 1.37 nm. The impact of Pd NP size on hydrogen evolution reaction (HER) activity was elucidated. Among the fabricated composites, Pd-MoS2 exhibits the best HER performance, attributed to its smallest Pd NP size (0.81 nm). It shows an overpotential of 70 mV at a current density of 10 mA cm−2, along with a Tafel slope of 43 mV dec−1. These HER performance metrics surpass those of most Pd-decorated 2D catalysts.
研究领域:
材料科学
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纳米技术
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电化学
·
催化
✓ 已验证
DOI
高影响因子
CHINESE CHEMICAL LETTERS
·
2019
·
IF 3.839
Tong Guo,Lina Wang,Sen Sun,Yan Wang,Xiaoling Chen,Kangning Zhang,Dongxia Zhang,Zhonghua Xue,Xibin Zhou
A novel three-dimensional (3D) layered MoS 2 @graphene functionalized with nitrogen-doped graphene quantum dots (MoS 2 @N-GQDs-GR) composites as an enhanced electrochemical hydrogen evolution catalyst. The few layered MoS 2 nanoflowers supported on N-GQDs-GR surface were elaborately fabricated by one-pot hydrothermal method, which MoS 2 and N-GQDs-GR exist in a bonding manner of Mo-N. In addition, due to the layered MoS 2 sheet edge exposes more hydrogen evolution active sites and N-GQDs-GR have high conductivity, the composites exhibit prominent electrocatalytic activity with a low overpotential 99 mV, a small Tafel slope 49.3 mV/dec. Therefore, that the current work will develop HER catalysts may replace Pt.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Jingwen Ma,Ruiting Wang,Tianai Zhang,Ying Tian,Jinhao Liu,Junbin Li
Urea-assisted hydrogen production is an emerging hydrogen production technology that offers a new approach to the efficient and clean production of hydrogen energy. The low energy consumption urea oxidation reaction replaces the high energy consumption oxygen evolution reaction (OER), significantly reducing the energy consumption of hydrogen production and achieving the resource utilization of pollutants in wastewater (including urea). It is expected to become an important pathway for green hydrogen production with both economic and environmental benefits. The novel composite catalyst Ru/NiMoOx@NC, prepared by supporting ruthenium on a nitrogen-doped carbon-coated nickel-molybdenum oxide support, exhibits highly efficient bifunctional catalytic activity, enabling it to efficiently catalyze the hydrogen evolution reaction (HER) and promote the urea oxidation reaction (UOR). Specifically, the introduction of trace ruthenium synergizes with the nickel-molybdenum bimetallic oxide to accelerate H 2 generation. The nitrogen-doped carbon substrate enhances the catalyst's electrical conductivity. Additionally, the incorporation of Mo reduces CO poisoning of Ni active sites during the UOR, further to enhance the catalyst's stability. By varying the loading of Ru, materials with optimal and superior properties are obtained. The Ru/NiMoO x @NC catalysts demonstrate excellent UOR (1.37 V vs. RHE@25 mA cm −2 ; 1.39 V vs. RHE@100 mA cm −2 ) and HER (−98 mV@25 mA cm −2 ) performance under alkaline conditions. The current density of the Ru/NiMoOx@NC electrode remains almost unchanged after cyclic voltammetry (CV) tests and chronoamperometric durability tests, exhibiting excellent catalytic stability. In this system, Ru/NiMoOx@NC serves as both the anode and cathode of the urea-assisted hydrogen production battery, which only requires a voltage of 1.56 V to achieve an output current density of 50 mA cm −2 and demonstrates excellent overall water electrolysis stability. This work provides new insights for the design of bifunctional catalysts for urea-assisted hydrogen production.
研究领域:
能源技术
·
催化
·
材料科学
·
电化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Hao Wu,Xian Jiang,Jingyu Lu,Yibo Li,Xinyan Li,Guidong Ju,Rengui Li,Jing Zhang
The hydrogen evolution reaction (HER) in alkaline water electrolysis faces significant kinetic and thermodynamic challenges that hinder its efficiency and scalability for sustainable hydrogen production. Herein, we employed an in-situ synthesis strategy to incorporate H atoms into the PdRu alloy lattice to form H Inc -PdRu electrocatalyst, thereby modulating its electronic structure and enhancing its alkaline HER performance. We demonstrate that the incorporation of H atoms significantly improves electrocatalytic activity, achieving a remarkably low overpotential of 25 mV at 10 mA cm –2 compared with the Pd, Ru and PdRu catalysts while maintaining robust catalyst stability. Operando spectroscopic analysis indicates that H insertion into the H Inc -PdRu electrocatalyst enhances the availability of H 2 O* at the surface, promoting water dissociation at the active sites. Theoretical calculations proposed that the co-incorporating H and Ru atoms induces s-d orbital coupling within the Pd lattices, effectively weakening hydrogen adsorption strength and optimizing the alkaline HER energetics. This work presents a facile approach for the rational design of bimetallic electrocatalysts for efficient and stable alkaline water electrolysis for renewable hydrogen production.
研究领域:
电催化
·
氢能
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材料科学
·
可再生能源
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Bing Hao,Manyuan Gan,Jingjing Guo,Guoshen Li,Yanhui Song,Yongqing Shen,Bingshe Xu,Peizhi Liu,Junjie Guo
The rational design and fabrication of 2D heterojuctions are proven a promising strategy for boosting the performance of electrocatalysts. Although 2D platinum diselenide (PtSe 2 ) exhibits catalytic activity for hydrogen evolution reaction (HER), the catalytic performance is still unsatisfactory due to its inert basal plane, wide bandgap, and poor electron transfer ability. Herein, a new strategy is reported to construct PtSe 2 /PtCo heterojunctions by partial selenization of PtCo alloy for high-efficiency HER electrocatalyst, which exhibits a low overpotential of 38 mV at the current density of 10 mA cm −2 , a small Tafel slope of 22 mV dec −1 , and a superior stability over 24 h and 1000 cycles. The outstanding HER activity of the catalyst arises from the strong electronic interactions between PtSe 2 and PtCo in the heterojunctions, which induce electron transferring from PtSe 2 to PtCo and the d-band center down shifting, and thus optimize the H * adsorption/desorption. This work provides a novel strategy for constructing highly efficient heterostructure electrocatalysts, which facilitates the applications of hydrogen energy conversion.
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
危险品化学品经营许可证（带存储）