ACS Applied Materials & Interfaces
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2025
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IF 8.2
Yue Liu,Wei Peng,Hancheng Ma,Jinsai Tian,Kao Wang,Zhaobo Zheng,Lin Xu,Yao Ding
Metal–organic frameworks have aroused growing interest in the research of energy conversion and storage. However, their specific configuration, especially the coordination environment of metal active sites, has not been well designed. Their role in regulating the structural reconstruction of pre-electrocatalysts remains ambiguous. Herein, this work reports a dual-ligand strategy to design a Ni-MOF with asymmetric Ni–O coordination, named Ni–BDC–DOBDC, which occupies unsaturated Ni sites and strengthens Ni–O bonds. As inspected by X-ray absorption near edge structure as well as a series of in situ and ex situ characterizations, this special Ni–O coordination contributes to Ov-NiOOH with rich oxygen vacancies during fast self-reconstruction at a lower potential. Moreover, theoretical results reveal that Ni sites in Ov-NiOOH occupy a higher d-band center, a lower adsorption energy barrier, and a more electronic negative surface in the oxygen evolution reaction, leading to good electrocatalytic performance. Overall, Ni–BDC–DOBDC catalysts exhibit a low overpotential of 202 mV at 10 mA cm–2 and outstanding stability within 240 h. The insights in this work pave the way for high-performance MOF-based catalysts by regulating their self-reconstruction kinetics through a new aspect of asymmetric ligand engineering.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
Materials Chemistry Frontiers
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2024
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IF 6
Yuru Zhou,Jing Hu,Yinan Liu,Wenyu Fan,Panpan Tao,Rui Yang,Haitao Huang,Xun Cao,Haijin Li,Siwei Li
Designing noble metal-free electrocatalysts remains a challenge for the oxygen evolution reaction (OER) in alkaline solutions. In this study, we present a facile electrodeposition approach coupled with an in situ anodic oxidation method to synthesize NiOOH–MnS/NF on nickel foam (NF), successfully creating NiOOH–MnOOH/NF heterojunctions to boost OER performance under alkaline conditions. The heterojunction's synergistic effect significantly modulates the adsorption energy of the rate-determining step (RDS), thereby enhancing the intrinsic electrocatalytic activity of the NiOOH–MnOOH/NF electrocatalyst. Furthermore, the introduction of SO42− leads to a variable degree of electron loss in both Mn and Ni, reducing adsorption strength of the OER intermediates and thus optimizing reaction kinetics. The as-prepared NiOOH–MnOOH/NF electrocatalyst demonstrates exceptional OER performance in 1.0 M KOH, achieving a current density of 100 mA cm−2 with a Tafel slope of 52.3 mV dec−1 and a minimal overpotential of 391 mV. Utilizing NiOOH–MnOOH/NF as a bifunctional electrode for overall water splitting (OWS), the system operates at a low potential of 1.66 V at 10 mA cm−2, showcasing its excellent durability. This work offers novel insights and promising prospects for the advancement and practical application of non-precious metal electrocatalysts in the field of electrocatalytic water splitting.
研究领域:
电化学
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材料科学
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催化
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能量转换与存储
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Junpu An,Hongchen Liu,Fan Yang,Kexin Wei,Chunhui Yu,Siyuan Sun,Yang Sun,Qing Guo,Jianfeng Wang,Chenlin Wang,Jiahui Liu,Kuobo Wang,Yongfeng Li
Nickel-based catalysts show great potential as promising candidates for the electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF). However, the limited adsorption capacity of nickel-based catalysts for OH – and HMF limits their further development. In this study, amorphous Fe/NiOOH-SO x was generated from nanosheets (Fe/NiOOH-Ni 3 S 2 ), which was pre-fabricated on nickel foam via pre-reconstruction and anionic regulation strategy. The optimized catalyst Fe/NiOOH-Ni 3 S 2 demonstrated exceptional activity in the HMF oxidation reaction (HMFOR) with a current density of 10 mA cm −2 at 1.32 V vs RHE, accompanying with the 98.9 % HMF conversion, 97.8 % 2,5-Furandicarboxylic acid (FDCA) selectivity, 96.8 % Faraday efficiency, and stability for ten cycles. The incorporating amorphous FeOOH reduces the electron density around Ni, promoting the formation of high-valent Ni spices. Meanwhile, the SO x combined with amorphous hydroxy nickel oxide provides unsaturated sites, which enhances the adsorption capacity of HMF. Density functional theory (DFT) computations reveal that the designed amorphous Fe/NiOOH and surface-adsorbed SO x collectively modulate the electronic structure of the catalyst, causing an upwards shift of the NiOOH d-band center and enhancing adsorption capacities for both HMF and OH – . This study proposes the adsorption enhancement mechanism of regulating electronic structure and offers a rational strategy for HMFOR electrocatalysts.
研究领域:
催化化学
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材料科学
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可再生能源
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
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IF 2.7
Yuxing Lian,Mengqin Zheng,Suhua Li,Wenqiang Lai,Dianping Tang,Youxiu Lin
A colorimetric and photothermal dual-mode detection method based on β-NiOOH nanozyme-3,3',5,5'-tetramethylbenzidine (TMB) system was established for Chloramphenicol (CAP) content in fruit juice. Here, a novel nanozyme β-NiOOH with high oxidase-like activity can directly and effectively catalyze the oxidation of colorless TMB to blue color TMB oxidation (oxTMB) without the presence of H2O2. Using a competition-type immunoassay, the oxTMB can induce not only a increase in absorption peak intensity but also a photothermal effect under 808 nm laser irradiation, achieving dual-mode detection of CAP. The increase of absorbance at 652 nm and the increase of temperature generated by photothermal conversion are linearly correlated with the CAP content. Under the optimal conditions, the dual-mode detection shows a low limit to 0.0056 ng/mL for the colorimetric method, and 0.0016 ng/mL for photothermal method. Moreover, the developed colorimetric and photothermal dual-mode immunobiosensor is successfully used to detect CAP in fruit juice with an acceptable recovery rate between 93.387% and 118.514%. This method has good repeatability, specificity, and accuracy, and provides an efficient approach for real-time detection of CAP in food safety analysis and detection platform.
研究领域:
食品科学
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免疫分析
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纳米技术
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产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
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2025
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IF 7.9
Ming Chen,Wen-Da Zhang,Qingna Gong,Xiangkun Zhang,Jiangyong Liu,Xiaoping Yang,Jing Wang,Xiaodong Yan
Urea oxidation reaction (UOR) has a lower thermodynamic potential compared to the oxygen evolution reaction, making it an effective alternative method for accelerating hydrogen production through water electrolysis. Currently, metal doping and heterostructure construction strategies have been shown to enhance UOR performance. However, these methods may introduce complexities, hindering the understanding of reaction mechanisms and the optimization of catalysts. In this study, thiol ligand is employed to modify Ni layered double hydroxide (Ni LDH), which increases the valence state of Ni. The thiol ligand modified Ni LDH achieves a current density of 100 mA cm −2 at 1.43 V, with a Tafel slope of 23.3 mV dec −1 . In situ Raman spectroscopy further demonstrates that the surface thiol ligand of Ni LDH facilitates the formation of Ni 3+ active sites, which is further confirmed by DFT calculation. The thiol ligand modification also enhances the electrochemical stability of Ni LDH. Our work provides an effective strategy for designing highly efficient and electrochemical stable UOR catalysts and highlights the broad potential of ligand modification in electrocatalysis.
研究领域:
材料科学
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电化学
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DOI
高影响因子
JOURNAL OF POWER SOURCES
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2020
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IF 8.247
Jing Li,Feng Li,Jun Jin
Hematite can be used as an efficient photoanode for solar water oxidation , but its oxygen evolution kinetics are quite slow. Herein, we developed an efficient hole transport photoanode via the in situ growth of ultrathin Fe-doped NiOOH on fluorine-doped hematite arrays using a natural growth strategy. The resulting FeNiOOH/F–Fe 2 O 3 photoanode showed a high charge separation and injection efficiency. It achieved a stable photocurrent density of 2.52 mA cm −2 at 1.23 V vs. RHE, which was approximately 4.1-fold higher than that of pristine α-Fe 2 O 3 . Systematic studies revealed that the excellent photoelectrochemical activity was due to heteroatom doping and interactions between the co-catalyst (FeNiOOH) and F–Fe 2 O 3 . Fe doping primarily changed the lattice strain of the co-catalyst, while F doping decreased surface charge recombination and enhanced the intrinsic conductivity of hematite by increasing the carrier density. An ultrathin, amorphous layer of FeNiOOH further accelerated photogenerated hole extraction and the water oxidation kinetics. This work provides a method to produce new, cost-effective photoanodes for clean hydrogen production .
研究领域:
材料科学
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可再生能源
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光催化
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
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2025
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IF 9.5
Gouda Helal,Zhenhang Xu,Wei Zuo,Jun Qian,Gongzhen Cheng,Pingping Zhao
Transition metal-based electrocatalysts undergo electrochemical surface reconstruction to generate metal oxy-hydroxide-based hybrids, which regard the actual active sites for the oxygen evolution reaction (OER). Many efforts have been devoted to understanding the electrochemical surface reconstruction, but there is rare research to identify the origin of improved OER performance derived from the substrate. Herein, we reported the electrochemical synthesis of an amorphous γ-NiOOH surface layer on NiFealloy/NiFeN pre-catalysts for efficient water oxidation. However, the conversion of β-NiOOH to γ-NiOOH is a thermodynamically unfavorable process, resulting in much higher applied potential to drive the reaction and subsequently catalyze OER.We identified that the NiFe-bimetallic active sites can promote the OER catalytic activity more than the Ni-monometallic active sites. Besides, nitrogen can reduce the potential required to generate γ-NiOOH OER-active sites from β-NiOOH and generate the NO3- anion, which promotes the formation of γ-NiOOH. The electrochemical analysis and in situ spectroscopic approaches, including cyclic voltammetry (CV), linear sweep voltammetry (LSV), and Raman, reveal that Ni species in NiFealloy/NiFeN are more thermodynamically favorable to form γ-NiOOH than in Nialloy/NiN and NiFeLDH. Beside the electrochemical behavior, X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HRTEM), and bode plots further demonstrate that Fe doping and nitrogen significantly increase the electrochemically active sites. Additionally, DFT calculation results show that the electronic structure of the catalysts is modulated by Fe doping, and the surface reconstruction optimized the adsorption energy of oxygen-containing species and enhanced the OER catalytic activity. This work provides a new design for constructing transition metal-based electrocatalysts for water oxidation.
研究领域:
电化学
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材料科学
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催化化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xin Guo,Longyu Qiu,Menggang Li,Fenyang Tian,Xue Ren,Sheng Jie,Shuo Geng,Guanghui Han,Yarong Huang,Ying Song,Weiwei Yang,Yongsheng Yu
Nickel sulfide (Ni 3 S 2 ) is a highly promising electrocatalyst for urea oxidation reaction (UOR), and NiOOH formed by the surface phase transition of Ni 3 S 2 during UOR is the ideal catalytic active species. However, the strong covalent bonds of Ni 3 S 2 hinders the generation of NiOOH, limiting the further improvement of UOR activity. Herein, the Ni 3 S 2 @Ni 3 P core–shell nanorods have been constructed by an in-situ surface phosphating method to boost UOR performance, realizing high catalytic activity (100/1000 mA cm −2 at 1.36/1.49 V vs . RHE, respectively) and a rapid kinetics (19.13 mV dec -1 ). The Ni 3 P on the surface of Ni 3 S 2 can rapidly form highly active γ-NiOOH with low energy consumption, and the formed Ni 3 S 2 @γ-NiOOH accelerates proton-coupled electron transfer (PCET) kinetics through reducing the energy barrier of urea dehydrogenation process, thereby enhancing UOR intrinsic activity. In addition, we also demonstrate a Ni 3 S 2 @Ni 3 P//Ni 3 S 2 @Ni 3 P urea electrolysis device with low voltages of 1.54 and 1.69 V at current densities of 100 and 500 mA cm −2 , respectively. This work proposes an efficient strategy to accelerate the generation of NiOOH on the surface of Ni 3 S 2 during UOR electrocatalysis, revealing the enhanced UOR mechanism of Ni 3 S 2 @Ni 3 P, which can promote the development of urea-assisted hydrogen production .
研究领域:
电化学
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催化材料
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能源转换与储存
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产品关联
DOI
高影响因子
Small
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2024
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IF 13
Feng Li,Shiyuan Xu,Xueru Zhao,Guorui Ma,Zhulin Niu,Xing Zhong,Jing Li
Fe-doped NiOOH electrocatalysts have attracted wide interest for the exceptional oxygen evolution reaction (OER) performance, but the precise role of Fe doping on the improved intrinsic activity remains unclear. Herein, the molecular probe technique combined with density functional theory calculation is used to reveal the influence of the Fe atom on the rate-determining step of the OER reaction, where the pre-catalyst of hierarchical self-supporting NiFe layered double hydroxide [LDH] nanosheets equipped on nickel foam (NiFe LDH/NF) is generated via a facile and industrially well-matched one-pot corrosion method. The physical characterization results reveal the reconstruction of NiFe LDH into Fe-doped NiOOH for promoted OER, which has a lower OH* adsorption energy with fast subsequent steps that help in obtaining an improved charge injection efficiency compared to NiOOH. In addition, more exposed electroactive species and facile delivery of mass/electron inside the catalytic procedure actually have a high-quality contribution to the outstanding catalytic activity. Therefore, the NiFe LDH 36 /NF electrocatalyst provides high catalytic activities of 241 and 320 mV at 10 mA cm −2 toward the OER and overall water-splitting in 1 m KOH. This work provides a promising avenue for the rational design of durable self-supporting electrodes toward large-scale water splitting.
研究领域:
材料科学
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电化学
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催化反应
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2021
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IF 3.995
Shaohua Wang,Ping Yang,Xiangfei Sun,Lina Feng,Congcong Jin,Menglei Ren,Honglong Xing,Jianjun Shi
Because of their low synthesis cost, large specific surface area, and good energy storage performance, microporous metal-based composites have been widely used in supercapacitors and the hydrogen evolution reaction (HER). Flower-like Ni foam@ (@, coating) NCo 2 O 4 @Ni(OH) 2 /NiOOH (NF@NCO@NOH) composites were synthesized through a simple solvent-controlled method and following an electrochemical deposition process. The as-synthesized composites benefit from high specific area, a hierarchical porous structure, and the synergistic effect of Ni and Co, showing a high area-specific capacitance of 23.75 F cm −2 at a continuous current of 5 mA cm −2 . The assembled asymmetric supercapacitor exhibits an energy density of 125 Wh kg −1 at a power density of 6.24 kW kg −1 . Furthermore, 84.1% of the capacity was retained after 10,000 cycles, suggesting the sample has excellent electrochemical stability. Moreover, an overpotential of 162 mV at a current density of 10 mA cm −2 and a Tafel slope of 95 mV dec −1 were obtained in the HER measurement, indicating that the as-synthesized flower-like electrode material possesses potential applications in the HER.
研究领域:
材料科学
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能源存储与转换
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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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
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电化学
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催化化学
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能源工程
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工业废水处理
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Tao Chen,Jiaxing Song,Menglei Xu,Zaifang Li
Urea-assisted hydrogen production can effectively improve the overall reaction rate, but achieving industrial-scale current density and long life is still a huge challenge. Herein, Vo-NiMoOOH/NF was prepared by hydrothermal-selenization-electrochemical reconstruction, which can achieve the industrial-grade current density of ∼860 mA cm −2 in an H-type reaction cell at 1.5 V (vs. RHE). A series of characterizations and DFT calculations reveal that the presence of oxygen vacancies and electrophilic-nucleophilic sites improves the D-band center of Ni, reduces the oxidation potential of Ni, accelerates the reconstruction of the catalyst, and inhibits the oxygen evolution reaction. Electrocatalytic urea oxidation coupled with hydrogen production was achieved in a two-electrode flow cell utilizing Vo-NiMoOOH/NF as a bifunctional catalyst. The current density of 1 A cm −2 at a cell voltage of 2.71 V and stable operation for more than 150 h at a current density of 500 mA cm −2 were realized, exhibiting excellent catalytic activity and stability.
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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纳米催化
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电化学工程
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产品关联
DOI
高影响因子