RARE METALS
·
2025
·
IF 11
Cheng-Feng Yi,Jing-Wen Li,Jia-Rui Li,Bing-Chuan Xue,Xing Lin,Zhi-Gang Liu
en Ni 3 S 2 has emerged as a promising catalyst for the electrochemical oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), driven by its distinctive physicochemical properties. However, its practical catalytic efficiency is severely hindered by abundant electrochemically inactive surface sites and poor electronic conductivity. To overcome these challenges, an N,W-cooperative modulation of Ni 3 S 2 catalyst (N,W-Ni 3 S 2 ), featuring an engineered crystalline-amorphous heterostructure, is designed, utilizing 5,10,15,20-tetraphenylporphine (TPP) as the N source. This innovative architecture integrates W-doped crystalline Ni 3 S 2 and N-doped amorphous carbon, which synergistically enhances charge transport and induces interfacial charge polarization, substantially boosting catalytic activity. The optimized N,W-Ni 3 S 2 demonstrates unprecedented electrocatalytic performance for the oxidation of HMF to FDCA, achieving 100% HMF conversion, 97% FDCA yield, and 97% Faradaic efficiency, with over 95% retention in both FDCA yield and Faradaic efficiency across 10 consecutive cycles. Theoretical calculations and experimental results unveil that N incorporation exerts a more profound influence than W in reshaping the electronic landscape of Ni 3 S 2 , triggering an asymmetric electron redistribution at the heterogeneous interface. This unique electronic perturbation depletes the electron density around Ni active sites, creating an electron-deficient state that dramatically promotes the in situ generation of NiOOH as the true active species. Furthermore, the tailored electronic environment significantly lowers the energy barrier for the rate-determining step in the oxidation pathway, thereby enabling near-quantitative FDCA production with high efficiency. 摘要 zh Ni 3 S 2 凭借其独特的物理化学性质,已成为一种极具前景的催化剂,可用于将生物质衍生的5-羟甲基糠醛(HMF)电化学氧化为2,5-呋喃二甲酸(FDCA)。然而,其实际催化效率因大量电化学惰性表面位点和较差的电子导电性而受到严重阻碍。为解决这些问题,本研究设计了一种具有工程化晶态-非晶态异质结构的Ni 3 S 2 催化剂的氮、钨协同调控体系(N,W-Ni 3 S 2 ),并以5,10,15,20-四苯基卟啉(TPP)作为氮源。这种创新结构整合了钨掺杂的晶态Ni 3 S 2 与氮掺杂的非晶碳,二者协同增强电荷传输并诱导界面电荷极化,显著提升了催化活性。优化后的N,W-Ni 3 S 2 在HMF氧化生成FDCA的反应中表现出优异的电催化性能:HMF转化率达100%,FDCA产率达97%,法拉第效率达97%; 在10次连续循环中,FDCA产率和法拉第效率均保持在95%以上。理论计算与实验结果表明,在重构Ni 3 S 2 的电子结构方面,氮掺杂比钨掺杂的影响更为显著,可在异质界面处引发不对称的电子重新分布。这种独特的电子扰动会降低Ni活性位点周围的电子密度,形成缺电子状态,从而显著促进真正活性物种NiOOH的原位生成。此外,这种定制化的电子环境大幅降低了氧化路径中决速步的能垒,进而实现了高效且接近定量的FDCA生成。
研究领域:
电催化
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可再生能源
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生物质转化
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材料化学
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可持续化学
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高影响因子
FUEL
·
2025
·
IF 7.5
Xin Zhang,Xiangyun Sun,Li Li,Xinli Zhang,Ao-Bing Wang,Huijuan Xu,Lijun Gao,Yaohui Gao,Hui Liu
Developing low-cost, highly efficient and stable non-noble metal-based electrocatalysts for the hydrogen evolution reaction (HER) is crucial for promoting large-scale alkaline water electrolysis. Here, we report a novel self-supporting Ni(OH) x /Mo-Ni 3 S 2 nanosheet heterostructure grown on nickel foam, demonstrating outstanding catalytic performance for alkaline HER. This heterostructure electrocatalyst exhibits an exceptionally low overpotential of just 33 mV at a current density of 10 mA cm −2 in 1 M KOH solution, surpassing commercial Pt/C catalyst. Moreover, it can operate continuously for 300 h at a high current density of around 130 mA cm −2 . Both experimental and theoretical calculations show that strong electronic coupling at the heterojunction interface optimizes the adsorption energy of molecular water and hydrogen on active sites, thereby enhancing the intrinsic activity. This work offers novel insights for designing high-performance alkaline HER electrocatalysts through coupling doping and heterostructure engineering.
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高影响因子
Small
·
2024
·Vol. 20
·期 26
·2310387
·
IF 13
Wei Luo,Yanli Yu,Yucheng Wu,Wenbin Wang,Yimin Jiang,Wei Shen,Rongxing He,Wei Su,Ming Li
Rational design of heterostructure catalysts through phase engineering strategy plays a critical role in heightening the electrocatalytic performance of catalysts. Herein, a novel amorphous/crystalline (a/c) heterostructure (a-CoS/Ni 3 S 2 ) is manufactured by a facile hydrothermal sulfurization method. Strikingly, the interface coupling between amorphous phase (a-CoS) and crystalline phase (Ni 3 S 2 ) in a-CoS/Ni 3 S 2 is much stronger than that between crystalline phase (c-CoS) and crystalline phase (Ni 3 S 2 ) in crystalline/crystalline (c/c) heterostructure (c-CoS/Ni 3 S 2 ) as control sample, which makes the meta-stable amorphous structure more stable. Meanwhile, a-CoS/Ni 3 S 2 has more S vacancies (S v ) than c-CoS/Ni 3 S 2 because of the presence of an amorphous phase. Eventually, for the oxygen evolution reaction (OER), the a-CoS/Ni 3 S 2 exhibits a significantly lower overpotential of 192 mV at 10 mA cm −2 compared to the c-CoS/Ni 3 S 2 (242 mV). An exceptionally low cell voltage of 1.51 V is required to achieve a current density of 50 mA cm −2 for overall water splitting in the assembled cell (a-CoS/Ni 3 S 2 || Pt/C). Theoretical calculations reveal that more charges transfer from a-CoS to Ni 3 S 2 in a-CoS/Ni 3 S 2 than in c-CoS/Ni 3 S 2 , which promotes the enhancement of OER activity. This work will bring into play a fabrication strategy of a/c catalysts and the understanding of the catalytic mechanism of a/c heterostructures.
研究领域:
材料科学
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电化学
·
催化化学
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纳米材料
·
能源材料
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.3
Guilian Li,Jintong Guo,Daming Yang,Hongji Xu,Linglong Hu,Shuo Geng,Ming Feng
Sluggish oxygen evolution reaction (OER) kinetics impede alkaline electrolysis. Here, vertically aligned Ru-decorated, Fe-doped Ni 3 S 2 nanowire arrays on Ni foam (Ru-NFS) are synthesized via a one-step hydrothermal route. Distinct from conventional Ni 3 S 2 →NiOOH systems, we operate in a low-Ru, Fe-co-modulated regime where Ru remains S-ligated and highly dispersed, evidenced by the absence of Ru-Ru scattering in EXAFS. This coordination accelerates NiOOH formation, enhances charge transfer, and mitigates Ru loss, yielding Ru-normalized activity beyond single-modulated controls. In 1.0 M KOH (iR-corrected), Ru-NFS requires only 206 and 245 mV to reach 10 and 100 mA cm -2 , respectively, and sustains stable operation. Mechanistically, COHP analysis shows that Fe substitution and, more strongly, Ru incorporation progressively weaken Ni-S bonds in the precursor, enabling rapid anodic reconstruction to NiOOH. On the reconstructed surface, DOS/PDOS reveal a d-manifold shifted toward EF with increased states, implying higher hole availability and optimized M-O covalency for coupled proton-electron transfer. DFT-CHE at 1.23 V (RHE) identifies *O→*OOH as the thermodynamic RDS, with ΔG reduced from 0.70 eV (NiOOH) to 0.48 eV (Fe-NiOOH) and 0.38 eV (Ru,Fe-NiOOH). Overall, Ru-Fe co-modulation couples reconstruction control with adsorbate-binding optimization, providing a blueprint for robust high-rate OER anodes.
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高影响因子
LANGMUIR
·
2026
·
IF 4.4
Xinya Ren,Taolue Liu,Fengguang Wang,Hao Li,Zifeng Huang,Yuling Li,Jinxuan Liu,Yu Wei,Yan Gao
Electrochemical water splitting is a crucial pathway for clean hydrogen production, but hydrogen evolution reaction (HER) electrodes often suffer from poor performance in alkaline conditions due to sluggish kinetics and weak durability. In this work, ammonium tetrathiomolybdate ((NH4)2MoS4) is used as a dual-functional precursor to transform Ni(OH)2 nanosheets into 3D Mo–Ni3S2 nanostructures. The fabricated electrode, Mo–Ni3S2/Nickel Foam, with an enlarged electrochemical active surface area, exhibits a low overpotential of 166 mV at 100 mA cm–2 in 1 M KOH and outstanding durability (>300 h). When integrated into anion-exchange membrane electrolyzers (AEMWE), it maintains stability for over 360 h at 500 mA cm–2. The enhanced performance could potentially be attributed to the hierarchical nanostructure that provides abundant active sites, and the in situ fabrication method ensures the durability of the electrode.
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Tariq Ali,Shahid Khan,Yiwei Li,Tariq Bashir,Bingjie Fang,Saleem Raza,Yeyuan Xiao
Urea-assisted water electrolysis offers a promising strategy for energy-saving hydrogen production with simultaneous wastewater valorization. Herein, a self-supported Fe-decorated Ni 3 S 2 nanosheet electrode on nickel foam (Fe–Ni 3 S 2 /NF) was prepared by hydrothermal growth followed by Fe electrodeposition. Structural characterization confirmed Fe introduction preserved the Ni 3 S 2 phase while inducing surface/electronic modulation. Electrochemically, Fe–Ni 3 S 2 /NF exhibited enhanced hydrogen evolution activity with overpotentials of 160, 222, and 259 mV at 10, 50, and 100 mA cm −2 , respectively (Tafel slope: 79 mV·dec −1 ). For urea oxidation, it delivered 10, 50, and 100 mA cm −2 at 0.97, 0.99, and 1.01 V, reducing the anodic potential by ∼0.62 V vs. OER at 100 mA cm −2 . A symmetric Fe–Ni 3 S 2 /NF || Fe–Ni 3 S 2 /NF electrolyzer required only 1.58–1.86 V for 10–100 mA cm −2 and operated stably for 50 h at 50 mA cm −2 , demonstrating a scalable noble-metal-free electrode for energy-efficient hydrogen production coupled with urea oxidation.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Yanyan Wu,Mingrun Song,Yingnan Dou,Wenjing Du,Hongru Hao,Yan Wang,Ying Li,Bo Wei
Although the availability of many nickel-based sulfides oxygen evolution reaction (OER) electrocatalysts with excellent intrinsic activity, very few of them perform well in anion exchange membrane water electrolysis (AEMWE). Their poor stability remains the core challenge in large-scale alkaline water electrolysis. In this work, the use of amorphous FeOOH nanoparticles is proposed as a modifier of Al doped Ni 3 S 2 (FeOOH/NiAlS) to develop robust OER electrode suitable for AEMWE. Under operation conditions, FeOOH protect the bulk sulfides from further corrosion, in turn effectively improves the catalyst utilization due to highly conductive property. Meanwhile, surface reconstructed Al-NiFeOOH serves as the actual active phase, monitored by in situ Raman and EIS. Density functional theory (DFT) reveals that Fe doping optimize their adsorption property, elongates the Ni O bond, and act as a new active site to augment OER activity. Specifically, the reconstructed FeOOH/NiAlS shows an ultra-low overpotential of 316 mV at 1 A cm −2 and high stability at 0.5 A cm −2 over 400 h. The corresponding AEMWE requires a cell voltage of only 1.72 V to reach 1 A cm −2 , while maintaining stable operation for 1400 h at 0.5 A cm −2 , providing a promising prospect for practical applications. Download: Download high-res image (103KB) Download: Download full-size image
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Van Nho Tran,Quoc-Nam Ha,Dong-Hau Kuo
Biomass-derived molecules, as renewable sources of organic carbon, are essential for selectively transforming into valuable chemicals and fuels, aiding in the mitigation of the energy dilemma brought on by the depletion of traditional fossil fuels. Owing to its unique chemical structure, furfural (FFR) is widely regarded as a key platform molecule derived from biomass, capable of being converted into various valuable chemicals, such as 2-furoic acid (2-FA). In this study, we design a CuWCe trimetal-doped Ni₃S₂ thin-film electrocatalyst that incorporates multivalent cations (Cu + /Cu 2+ , W 5+ /W 6+ , and Ce 3+ ) to enhance the economic feasibility of electrocatalytic FFR conversion to 2-FA for commercial use. We successfully synthesized an in situ grown nanoflower-like CuWCe-2 electrocatalytic material using a simple hydrothermal method. The catalyst achieved an FFR conversion efficiency of 79.8% to 2-FA, with a selectivity of 89.6%, at an FFR initial concentration of 35 mM. The 2-FA was produced at a high yield rate of 876 μmol·cm -2 ·h -1 and a faradaic efficiency (FE) of 90.1% at 1.45 V versus the reversible hydrogen electrode (RHE) in an H-cell setup.
研究领域:
电催化
·
可再生能源
·
材料科学
·
生物质转化
·
可持续化学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Nianwen Song,Jiangtao Qu,Bo Feng,Keyi Lv,Yanfei Wei,Xiaofei Yu,Lanlan Li,Xinghua Zhang,Xiaojing Yang,Rongkun Zheng,Yahui Cheng,Zunming Lu
Among non-precious metal catalysts, non-oxide materials often undergo surface oxidation under high-anodic potentials during the oxygen evolution reaction (OER), forming hydroxyl oxides or oxyhydroxides that serve as the true active phases with intrinsically higher activity. However, this structural transformation is frequently accompanied by surface relaxation, lattice distortion, or even partial collapse, leading to progressive degradation of catalytic stability, particularly under high-current-density operation, where long-term structural integrity is severely challenged. Enhancing the operational stability of such non-oxide catalysts is therefore a critical and unresolved challenge. In this work, we rationally doped Ti atoms into the Ni 3 S 2 lattice via a one-step solvothermal synthesis. Ti incorporation introduces low-coordinated metal sites that function as highly dispersed, atomically efficient active centers. These sites promote rapid deprotonation kinetics and lower the energetic barrier for O O bond formation, thereby significantly boosting intrinsic OER activity. The resulting catalyst delivers an overpotential of only 238 mV to achieve a current density of 10 mA cm −2 in 1 M KOH. Crucially, during electrocatalysis, the oxyphilic Ti dopants undergo controlled, sacrificial dissolution and act as “voltage buffers” that mitigate lattice strain and suppress irreversible oxidation of the Ni S framework under high anodic bias. This dynamic stabilization mechanism preserves the structural coherence of the catalyst, enabling stable operation at relevant current densities for over 400 h. Density functional theory (DFT) calculations corroborate the mechanism that confirms the preferential adsorption of OH* and O* intermediates at bridge and top sites associated with low-coordinated Ni atoms, and quantitatively reveal how Ti doping modulates the adsorption strength and coverage of key intermediates across applied potentials. Collectively, this study demonstrates a scalable, rational design strategy integrating targeted dopant selection, mechanistic understanding, and operando stabilization that advances non-oxide, non-noble metal catalysts toward practical water electrolysis applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Peng Zhou,Yaqiang Wu,Cong Wang,Huining Huang,Danning Xing,Yuanyuan Liu,Zeyan Wang,Peng Wang,Zhaoke Zheng,Hefeng Cheng,Ying Dai,Baibiao Huang
Tailoring the composition and structure of transition metal compounds via a simple method is a crucial step in the pursuit of high-performance electrochemical energy storage materials. Herein, we design and synthesize a Co modified Ni 3 S 2 (denoted as Co-Ni 3 S 2 ) electrode with a hierarchical structure by a simple one step sulfuration reaction from NiCo-LDH. Benefiting from both the hierarchical structure and the bimetallic composition, the developed electrode exhibits excellent electrochemical performances including ultrahigh specific capacitance (1826.4 F g −1 at 2 A g −1 ) and great rate capability (about 53.9% at 20 A g −1 ), which are much higher than that of NiCo-LDH precursor and monometallic Ni 3 S 2 electrode. Moreover, the energy storage device assembled with the Co-Ni 3 S 2 electrode and the activated carbon (AC) electrode exhibits superior energy density of 59.1 Wh kg −1 and 24.7 Wh kg −1 while maintaining the ultrahigh powder density of 1275.5 W kg −1 and 9.8 kW kg −1 , respectively. In addition, the device also displays an outstanding electrochemical stability (about 94.9% retention after 16,000 cycles).
研究领域:
材料科学
·
电化学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xinyu Wang,Xu Yu,Shuang Wu,Pinyi He,Fu Qin,Yongkang Yao,Jianliang Bai,Guojun Yuan,Lili Ren
The rational design of highly efficient and stable electrocatalysts for the oxygen evolution reaction (OER) is an urgent need but remains challenging for various sustainable energy systems. How to adjust the atomic structure and electronic structure of the active center is a key bottleneck problem. Accelerating the electron transfer process and the deep self-reconstruction of active sites could be a cost-effective strategy toward electrocatalytic OER catalyst development. Here, a crystalline–amorphous (c–a) coupled Ni3S2/NiPx electrocatalyst self-supported on nickel foam with an intimate interface was developed via a feasible solvothermal-electrochemistry method. The coupling interface of the crystalline structure with high conductivity and amorphous structure with numerous potential active sites could regulate the electronic structure and optimize the adsorption/desorption of O-containing species, ultimately resulting in high OER catalytic performance. The obtained Ni3S2/NiPx/NF presents a low OER overpotential of 265 mV to obtain 10 mA·cm–2 and a small Tafel slope of 51.6 mV·dec–1. Also, the catalyst with the coupled interface exhibited significantly enhanced long-term stability compared to the other two catalysts, with <5% decay in OER activity over 20 h of continuous operation, while that of Ni3S2/NF and NiPx/NF decreased by about 30 and 50%, respectively. This study provides inspiration for other energy conversion reactions in optimizing the performance of catalysts by coupling crystalline–amorphous structures.
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PubMed
高影响因子
LANGMUIR
·
2023
·
IF 3.9
Jie Ying,Zhen-Zhao He,Jiang-Bo Chen,Yu-Xuan Xiao,Xiao-Yu Yang
Many attempts have been made to enhance the relatively poor electrochemical activity of Ni3S2 for the oxygen evolution reaction (OER) by elevating the d-band center. Unfortunately, only limited success has been encountered thus far. Owning to the lower electronegativity and one less 3d electron relative to Ni, Fe shows great potentials in upshifting the overall d-band center of Ni3S2 when incorporating into its crystal structures. Herein, to enhance the intrinsic activity by elevating the d-band center, Ni3S2 nanosheets incorporated with suitable Fe content have been fabricated by a facile one-step solvothermal method. The obtained Fe-incorporated Ni3S2 catalyst exhibits an outstanding OER performance in alkaline media, only requiring 244 mV overpotential (with a reduction of 210 mV compared to Ni3S2) at 50 mA cm–2 in 1 M KOH and without obvious degradation after sustaining for a 60 h test at a voltage above 1.5 V. Ultraviolet photoemission spectroscopy and density functional theory calculations consistently demonstrate that the superior performance of Fe-incorporated Ni3S2 is attributed to the upshift of the d-band center on neutralizing the electron densities of Ni, which optimize greatly the adsorption energy of the intermediate (OOH*) in the rate-determining Volmer step.
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高影响因子
危险品化学品经营许可证（带存储）