Particuology
·
2022
·
IF 3.251
Chao Song,Yuhua Liu,Chengxiang Huang,Miao Liu,Nailin Yue,Zunhao Zhang,Zizhun Wang,Xu Zou,Wei Zhang,Weitao Zheng
Through inverted-design rather than modifying the generally-assumed S active sites in popular MoS 2 , we unlock the potential of Mo sites and successfully prepared novel MoS 2 @Ni 3 S 2 /NF core-shell nanospheres as a catalyst for the high-performance hydrogen evolution reaction (HER). The ΔG H at the Mo site is optimized via Ni 3 S 2 to achieve excellent HER activity. At low current densities, it has similar activity to the Pt/C. However, its performance is better than Pt/C at high density. Moreover, our catalyst shows a considerable stability at a variety of current densities for 50 h, promising to substitute noble metal catalysts in application of commercial alkaline electrocatalysts .
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
·
2023
·
IF 15.1
Su Yan,Xia Yang,Mengxiao Zhong,Weimo Li,Xiaojie Chen,Jiaqi Xu,Wei Chen,GuangTao Yu,Ce Wang,Xiaofeng Lu
In this study, a series of X-Rh (X = Fe, Co, Ni) alloy aerogels (AGs) are constructed via a galvanic replacement strategy. Due to the optimized electronic structure and the unique features of metal aerogel, the resultant Co AG-Rh500 electrocatalyst exhibits much better HER activity and robust stability than the benchmark commercial Pt/C catalyst in all-pH media. Theoretical result further reveals that the top sites of Co and Rh atoms in the (0 0 1) and (1 0 0) surfaces of the hybrid CoRh alloy systems can act as the active sites especially in an acidic condition, while the bridge and hollow sites on the (0 0 1) and (1 0 0) surfaces of CoRh alloy contribute a lot to the superior HER kinetics in alkaline and neutral electrolytes. Furthermore, the apparent electron transfer between Co and Rh atoms modulates the adsorption state of H*, thereby promoting the HER performance.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Xueyan Li,Chaojie Lyu,Dandan Cui,Senlong Zhang,Jiarun Cheng,Hanyu Guo,Chaojie Lyu,Yiming Liu
For the intrinsic limitations of CoP in alkaline water splitting (irrational electronic structure, poor conductivity, and agglomeration-caused low active site utilization), this work puts forward a bifunctional optimization strategy: "Fe-doping electronic modulation coupled with rGO support synergistic enhancement", and synthesizes the Fe-CoP@rGO composite catalyst (Fe-doped CoP nanoparticles anchored on rGO) via wet-chemical method and phosphidation. The introduction of Fe induces electron rearrangement by substituting Co atoms in CoP lattice significantly increases the proportion of highactivity Co 3+ sites and optimizes the adsorption energy barriers of *H/*OH intermediates. Meanwhile, the high conductivity of rGO constructs an efficient electron transport network, and its large specific surface area inhibits nanoparticle agglomeration through steric hindrance, enhancing the electrochemical active surface area (ECSA) twice that of pure CoP.Bifunctional catalytic performance tests show that Fe-CoP@rGO achieves low overpotentials of 86.2 mV (HER) and 285 mV (OER) at 10 mA cm -2 , which are significantly superior to those of CoP@rGO. When assembled into an overall water splitting device, it only requires 1.61 V to reach 10 mA cm -2 , with no performance degradation after 24 h of continuous operation in 1 M KOH and a Faraday efficiency close to 100%. This study provides a clear structure-activity relationship and a scalable optimization pathway for designing high-performance and stable non-noble metal bifunctional electrocatalysts through the synergistic effect of electronic structure modulation and support function enhancement
✓ 已验证
产品关联
DOI
高影响因子
Materials Science and Engineering B-Advanced Functional Solid-State Materials
·
2025
·
IF 4.6
Nazhen Zhang,Lijuan Ma,Jing Zang,Yue Gao,Yue Zhong,Songyang Sun,Yanwei Li,Yanhui Li
The exquisitely engineered multifunctional electrocatalysts for oxygen reduction reactions (ORR), hydrogen evolution reactions (HER) and oxygen evolution reactions (OER) hold significant importance in current research. In this work, layered porous C-FeNC-900 electrocatalyst has been successfully prepared using a NaCl induced pyrolysis strategy based on metal organic frameworks (MOFs). The presence of NaCl during the pyrolysis process not only effectively enhances the porous structures, but also promotes numerous Fe N x active sites and improves the degree of carbon graphitization. Due to the simultaneous construction of highly active Fe N x sites on the graded porous carbon skeleton, the electrochemical accessibility and corrosion resistance are improved. The prepared C-FeNC-900 electrocatalyst exhibits a half wave potential of 0.859 V for ORR in alkaline conditions, exceeds the half wave potential of Pt/C at 0.854 V. Moreover, the results demonstrate C-FeNC-900 has excellent stability, with an initial current density retention of 88.45 % after a durability lasting 10,000 s. At the same time, C FeNC-900 has possesses a potential of 1.67 V at a current density of 10 mA cm −2 during OER testing, with a Tafel slope of 209 mV. The C FeNC-900 also displays HER performance with potential of 405 mV and Tafel slope of 178.4 mV. This study provides a new perspective to construct multifunctional catalysts with well-designed structure for clean energy conversion technologies.
研究领域:
材料化学
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电化学
·
纳米催化
·
能源材料
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多孔材料科学
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可持续能源技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Ting Xiang,Kang Chen,Siqi Ni,Xijun Wang,Changlun Chen
The electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) offers an eco-friendly route to produce 2,5-furandicarboxylic acid (FDCA). Coupling this anodic reaction with the hydrogen evolution reaction provides a sustainable alternative to oxygen evolution reaction in water electrolysis, enhancing energy efficiency while generating green hydrogen. However, conventional nickel-based catalysts suffer from weak substrate adsorption and limited active-site utilization. Here, we introduce a ligand-engineered charge-transfer complex, Ni(TCNQ) 2 (H 2 O) 2 , in which π-conjugated TCNQ ligands enable strong π–π stacking with the furan ring of HMF to enrich substrate adsorption, while the electron-accepting nature of TCNQ mediates metal-ligand charge transfer to regulate the Ni 2+ /Ni 3+ redox couple. This dual function significantly accelerates reaction kinetics and stabilizes intermediates, enabling Ni(TCNQ) 2 (H 2 O) 2 to deliver 100 mA·cm −2 at 1.38 V and nearly 100 % FDCA yield. Mechanistic insights from X-ray photoelectron spectroscopy, operando Raman, and density functional theory (DFT) confirm that ligand-driven adsorption and electron interactions accelerate the catalytic process. DFT free-energy profiles further demonstrate that Ni(TCNQ) 2 (H 2 O) 2 smooths the reaction energy landscape, lowering the thermodynamic barriers compared with Ni(OH)₂. This work underscores the pivotal role of ligand engineering in tuning catalytic interfaces for efficient biomass electrooxidation and green hydrogen co-production in integrated renewable energy systems.
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Mutian Zhang,Ziying Ji,Xing Wang,Yulin Ouyang,Zening Yang,Siyuan Zhou,Miao Zeng,Wei Zheng,Jiajia Wang,Guobing Ying
Understanding the catalytic mechanisms of the alkaline hydrogen evolution reaction (HER) is essential for the rational design of efficient catalysts. In this work, Fe/Ni-doped Co 3 O 4 systems were investigated by combining DFT+U calculations with experimental validation. Theoretical simulations reveal that both dopants induce spin-state transitions in Co 3+ , tune orbital hybridization, and redistribute reaction energy barriers across elementary steps rather than uniformly lowering them on the Co 3 O 4 (110) surface. Hydrothermally synthesized Fe-Co 3 O 4 and Ni-Co 3 O 4 microflower spheres confirm these predictions: Ni doping lowers the overall reaction barrier by optimizing the electronic structure and adsorption energetics associated with high-spin Co 3+ , leading to a reduced onset overpotential, whereas Fe doping facilitates water dissociation via enhanced spin polarization, thereby lowering the rate-determining barrier and improving kinetics at high current densities. Further analyses identify reliable descriptors for different catalytic advantages: the overall reaction barrier, d -band center, and covalent bonding degree of water adsorption serve as indicators of thermodynamically favorable catalysts with low overpotential, whereas the rate-determining step barrier and d-p coupling are key descriptors of kinetically favorable catalysts with enhanced current-density performance. This study clarifies the step-specific roles of spin-state modulation and provides a framework for catalyst design based on energy barrier redistribution.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2026
·
IF 9.2
Yu Liao,Yaowei Liu,Yang Li,Linjuan Zhang,Jian-Qiang Wang,Sivaprakash Sengodan,Bingbing Niu,Guntae Kim
Carbon capture, utilization, and storage (CCUS) is recognized as a critical pathway for decarbonization, but current approaches are limited by energy-intensive operation and suboptimal conversion efficiency. In this context, the Zn-CO2 system holds immense promise for simultaneous electricity generation, green hydrogen production, and efficient CO2 utilization. However, further improvement of the overall system efficiency hinges on enhancing the hydrogen evolution reaction (HER) in quasi-neutral media. Herein, we report a Mn-doped cobalt phosphide (Mn-CoP/NF) catalyst grown on nickel foam via a facile one-step electrodeposition, designed to promote water dissociation and enhance HER activity in neutral electrolytes. Structural characterizations reveal that Mn doping induces an amorphous transformation with a cauliflower-like morphology, markedly increasing the electrochemical active surface area (ECSA) and exposing abundant active sites. XPS analysis further confirms that Mn functions as an electron donor, generating electron-rich Co/P surfaces that favor optimized adsorption of reaction intermediates. Kinetic analysis demonstrates that the incorporation of oxyphilic Mn substantially lowers the Tafel slope from 158.7 mV dec -1 to 62.0 mV dec -1 , evidencing accelerated water dissociation in the Volmer step. Density functional theory (DFT) calculations reveal that Mn incorporation lowers the water dissociation energy barrier and optimizes the hydrogen adsorption free energy (ΔGH*). Consequently, the Mn-CoP/NF catalyst exhibits outstanding HER activity in saturated KHCO3 solution, with an overpotential of 149.9 mV at 50 mA cm-2 , similar to commercial 1 mg cm-2 Pt/C (146.4 mV). Furthermore, the Zn-CO2 system assembled with Mn-CoP/NF as the HER electrode achieves a maximum current density of 378 mA cm -2 and sustains stable operation for over 300 hours at -100 mA cm-2 .
✓ 已验证
DOI
高影响因子
Carbon Energy
·
2026
·
IF 21.4
Liangmeng Ni,Aiyue Huang,Xin Feng,Zhijia Liu
Proton exchange membrane (PEM) electrolysis demands hydrogen evolution reaction (HER) cathodes that minimize precious-metal usage while remaining durable in strongly acidic media, yet improving Pt utilization and stability under reduced PGM loading remains challenging. Here, we develop a programmable nucleation pathway that uses in situ H* from formic acid (HCOOH) dehydrogenation at a Ru–Pd interface to gate reducing equivalents during nucleation. This enables site-confined Pt nucleation/immobilization and stabilizes a hydrogen-management interface for H* generation, relay, and recombination. The resulting Ru–Pd–Pt/C comprises uniformly dispersed ternary nanodomains (~2.46 nm). In 0.5 M H 2 SO 4 , Ru–Pd–Pt/C delivers η 10 = 12.24 mV, an apparent Tafel slope of 29.9 mV dec −1 from a unified 20–50 mV fitting window, and a PGM mass activity of 6.58 A mg PGM −1 at η = 50 mV. More importantly, membrane electrode assembly tests under identical assembly conditions show lower cell voltages than commercial 40 wt% Pt/C over 1–4 A cm −2 and stable operation at 1 A cm −2 . Density functional theory calculation shows Ru/Pd neighbors tune Pt toward near-thermoneutral H adsorption (ΔG H* = −0.19 eV), consistent with density of states/d-band shifts and the improved apparent HER response. This formation-stage programming offers a transferable framework for durable, low-PGM HER cathodes in acidic water electrolysis.
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yushi Han,Qin Yin,Shuo Geng
The development of the liquor industry urgently needs to solve the problem of wastewater treatment. The electrochemical oxidation method, with its advantages of high efficiency and environmental friendliness, has surpassed traditional processes. The low electro-oxidation potential of organic alcohols in wastewater (significantly lower than the oxygen evolution reaction, OER) endows it with dual value: it can replace the anode OER while simultaneously achieving pollutant degradation and driving the hydrogen evolution reaction (HER) at the cathode, achieving the synergy of “anode pollution control and cathode hydrogen production”. Based on this, this study constructed a Fe-NiOOH/NiMo/NF heterojunction catalyst, which, through the synergy of the efficient alcohol degradation ability of Fe-NiOOH and the excellent hydrogen evolution performance of NiMo, established a stable coupling system for wastewater degradation and hydrogen evolution at high current densities. Experiments confirmed that: Experimentally, the Fe-NiOOH/NiMo/NF anode delivers 200 mA cm −2 at 1.434 V vs. RHE; the NiMo/NF cathode reaches 20 mA cm −2 at an overpotential of 88 mV; and the full cell (Fe-NiOOH/NiMo/NF=|NiMo/NF) sustains 100 mA cm −2 for 100 h with only a 30 mV rise in voltage. Compared with the high-purity alcohol-based OER replacement scheme, using low-cost liquor wastewater as the anode reactant significantly reduces the cost of hydrogen production. The stable operation of this synergy system at high current densities provides a reliable technical path for the industrialized wastewater degradation and hydrogen production.
研究领域:
环境科学
·
电化学
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催化化学
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能源工程
·
工业废水处理
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Qi Qiu,Tao Wang,Linhai Jing,Kun Huang,Dabin Qin
Tetra-carboxylic acid based 3D porous MOFs 1 and 2 , named {[Co 2.5 (L)]·5H 2 O} n and 0.5{[Cu(L)]·2H 2 O} n (L = 4,4′-di(ethoxy)biphenyl-3,3′,5,5′-tetra-(phenyl-4-carboxylic acid)), bearing metal clusters have been facilely constructed by hydrothermal synthesis . Structural studies indicate that 1 presents a 3-nodal (4, 4, 8)-connected topology with the point notation of {4 4 .6 2 }2{4 8 .6 7 .8 13 }, while 2 shows a uninodal (4, 4)-connected network with point symbol of {4 4 .6 2 }. The pristine MOFs are directly utilized for electrocatalysis and poor HER activities are obtained in alkaline solution, which promote the further design and fabrication of a mixed-metal Co/Cu-MOF ( 3 ). As expected, 3 shows significantly improved performances for HER with overpotential of 391 mV (10 mA cm −2 current density), low Tafel slope of 94 mV dec −1 and long-term operation stability (14 h). More importantly, the direct utilization of 3 for accelerating OER also presents a fascinating performance in overpotential at 10 mA cm −2 current and durability. The above electrocatalytic performance of pristine 3 can be ascribed to the result of hybridizing strategy for constructing MOFs under hydrothermal procedure, which may favorably produces synergistic effect and more open metal sites. This work provides in-depth understanding of hybrid pristine MOFs for electrocatalysis.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2021
·Vol. 12
·期 1
·2102359
·
IF 29.368
Yuan Chang,Panlong Zhai,Jungang Hou,Jijun Zhao,Junfeng Gao
Faced with grave climate change and enormous energy demands, effective catalysts have become more and more important due to their significant effects on reducing fossil fuels consumption. The hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) by water splitting are feasible ways to produce clean sustainable energy. Here, atomic structures and related scanning tunneling microscope images of Se defects in PtSe 2 are systematically explored. The equilibrium fractions of vacancies under variable conditions are predicted in detail. In addition, it is found that the vacancies are highly kinetically stable, without recovering or aggregation. The Se vacancies in PtSe 2 can dramatically enhance the HER performance, comparing to Pt(111). It is also revealed that a PtSe 2 monolayer with Se vacancies is also a good OER catalyst. The excellent bipolar catalysis of Se vacancies is further confirmed by experimental measurements. A defective PtSe 2 made via direct selenization of Pt foil at 773 K using a chemical vapor deposition process is produced. It is shown that the HER and OER performance of defective PtSe 2 is much more efficient than Pt foils by a series of measurements. This work, with its compelling theoretical and experimental studies indicates PtSe 2 with Se defects is an ideal bipolar candidate for HER and OER.
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
Journal of the American Chemical Society
·
2025
·
IF 15.6
Ting Gao,Jie Gu,Changheng Yang,Rui Wang,Chan Wang,Pengfei Zhang,Jiatong Li,Xiaoyan Zheng,Yunmiao Fan,Puheng Yang,Xiufu Hua,Junfeng Hui,Huigang Zhang
Hydrogen is a promising clean energy carrier, yet the high energy demand of water electrolysis limits its widespread adoption. Catalysis is crucial to enhance the efficiency of hydrogen production and lower energy costs. However, conventional catalyst design guided by the d-band theory faces inconsistencies in predicting adsorption behavior, and the oxygen evolution reaction (OER) remains a major efficiency bottleneck. To address these challenges, we developed a strain-engineered Rh single-atom catalyst anchored on curved WS2 supported by carbon nanotubes (RhSA/WS2@CNT) to modulate the electronic structure. The resultant catalyst achieves an ultralow overpotential of 17.4 mV at 10 mA cm–2 for the hydrogen evolution reaction (HER) and a mass activity ∼65 times higher than that of commercial Pt/C. Mechanistic analysis reveals that the H* adsorption trend contradicts d-band theory predictions but is explained by orbital symmetry adaptation, where the strain-modulated dxz orbital plays a major role in governing adsorption energetics. Beyond catalyst design, the HER catalyst was coupled with a photocatalytic iodide oxidation reaction (IOR) to replace the OER and reduce the water-splitting voltage to 0.7 V. This study not only introduces a strain-engineering strategy to optimize single-atom catalysts but also demonstrates a coupled electro-photo system that enhances energy efficiency, offering an alternative approach for sustainable hydrogen production.
研究领域:
材料科学
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催化化学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）