ACS Applied Energy Materials
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2021
·
IF 6.024
Lin-Chang Liu,Hong-Lin Zhu,Yue-Qing Zheng
Ammonia borane (NH3BH3, referred to as AB) hydrolytic dehydrogenation is regarded as a feasible strategy for hydrogen production owing to its high hydrogen content, pollution-free nature, and high stability. Metal nitrogen-doped carbon materials (M-N-C) are considered as an ideal candidate support of catalysts with AB hydrolytic dehydrogenation due to the advantages of low cost, large specific surface area, rich defective site, and good chemical stability. In this work, tubular Ni@Ni-N-C was successfully synthesized by high-temperature pyrolysis, and then, Rh nanoparticles were decorated on the support Ni@Ni-N-C by impregnation and reduction to prepare a series of Rh/Ni@Ni-N-C. The best catalytic performance of catalysts is obtained using Ni@Ni-N-C with an Rh loading of 0.74 wt %, showing a turnover frequency as high as 782.18 min–1 and an apparent activation energy (Ea) as low as 25.86 kJ mol–1, which could be attributed to the strong interaction between Rh and the defective site of the support.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 16
·10169-10179
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IF 12.732
Fuzhen Zhao,Huicong Liu,Houyu Zhu,Xiaoyu Jiang,Liqun Zhu,Weiping Li,Haining Chen
Amorphous/amorphous heterostructures with a large surface area are theoretically anticipated to promote the alkaline hydrogen evolution reaction (HER) activity and stability. However, the growth, characterization and theoretical simulation of amorphous/amorphous nanostructured heterostructures are still challenging due to their atomic isotropy. Herein, a novel and simple strategy is developed to synthesize amorphous/amorphous Ni–P/Ni(OH)2 heterostructure nanotubes by immersing Zn@Ni–P nanowires grown by axial screw dislocation in alkaline solution. When used as an HER catalyst, the Ni–P/Ni(OH)2 nanotubes achieve considerably high electrocatalytic activity and decent stability. The significantly low overpotential of 54.7 mV at a current density of 10 mA cm−2 is among the best values reported for transition metal phosphides in alkaline solution. Density functional theory calculations indicate that the abundant defect structures of amorphous Ni–P would shift the Ni 3d band center toward the Fermi level, demonstrating an energy barrier decrease for H2 generation. Furthermore, the synergistic effect of amorphous Ni–P and Ni(OH)2 could significantly enhance H2O dissociation to supply sufficient protons for the HER.
研究领域:
材料科学
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电化学
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理论计算
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2015
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IF 2.999
Qingnan Wu,Ming Wen,Shipei Chen,Qingsheng Wu
Ni(OH) 2 /CNTs/Ni(OH) 2 lamellar-crossing-nanostructure with a single lamellar spacing of ∼5 nm was effectively constructed through two-phase-interface reaction process followed by the CNTs crossed among the lamellar-nanostructured Ni(OH) 2 . The resultant nanocomposite can offer large active surface areas and short diffusion paths for electrons and ions, and is investigated as a potential pseudocapacitor electrode material for electrochemical energy storage applications. Electrochemical data demonstrate that the as-prepared nanocomposite exhibits a high specific capacitance of ∼1600 F g −1 at the scan rate of 1 mV s −1 in 6 M KOH solution at normal pressure and temperature, which is great higher than Ni(OH) 2 (∼1200 F g −1 ). Furthermore, Ni(OH) 2 /CNTs/Ni(OH) 2 nanocomposite shows a higher energy density (∼125 Wh kg −1 , 2 A g −1 ) and has a slightly decrease of 5% in specific capacitance after 1000 continuous charge/discharge cycles.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
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2022
·Vol. 135
·期 5
·2533-2550
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IF 1.843
Chen Wei,Bao Zhichang,Zhou Zhiming
A series of non-precious bimetallic NiM x /SiO 2 (M = Zn or Co) catalysts with a fixed Ni loading of 5 wt% and different molar ratios of M/Ni (0.004–1.97) were prepared by glucose pyrolysis and applied to the selective hydrogenation of phenylacetylene. The properties of the catalysts were characterized by N 2 physisorption, CO chemisorption, ICP-OES, TGA, XRD, HRTEM, XPS, and DRIFTS. The activity and selectivity of the bimetallic catalysts could be tuned by varying the Zn/Ni and Co/Ni molar ratios, which were almost independent of the metal particle size (with a similar size of 4.1–5.5 nm), but predominantly determined by the geometric and/or electronic effects of the catalysts. Among all the catalysts studied, NiZn 0.05 /SiO 2 and NiCo 0.09 /SiO 2 presented higher selectivity to styrene (86.3% and 88.0%, respectively) at above 99% conversion of phenylacetylene. The high selectivity of the former was attributed to the geometric and electronic effects of the Ni–Zn alloy, while the latter was due to the geometric effect caused by the addition of Co. The activity and selectivity of NiCo 0.09 /SiO 2 were maintained during six consecutive cycles, indicating its good stability in the selective hydrogenation of phenylacetylene.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2024
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IF 5.5
Liang Ding,Roujia Zhang,Peng Zhao,Changsheng Qu
Based on the remediation challenges and practical needs of trichloroethylene (TCE)-contaminated groundwater, this study prepared an Ni-based composite electrode, Pd/Ni(OH) 2 /Ni foam (NF), and evaluates its electrocatalytic degradation effect on TCE in a groundwater environment. Under an applied voltage of –1.3 V versus Ag/AgCl, the TCE removal rate reaches 95% after 3 h of electrolysis. The introduction of Ni(OH) 2 nanoarrays accelerates the electron transport process, shortens the ion transport distance, and significantly increases the electron density of Pd. Furthermore, TCE is rapidly reduced by adsorbed hydrogen radicals on the Pd surface, and the ethane conversion rate reaches 62%. The experimental results show that the electrode can maintain a strong electrocatalytic activity over a wide pH range (3–9) and that it is not affected by common anions, such as Ca 2+ , HCO 3 - , SO 3 2- , or Cl - , in groundwater. Pd/Ni(OH) 2 /NF exhibits a high reactivity after six cycles of use. The remediation mechanism is studied by combining the microscopic characterization of materials, electrochemical activity testing, and process product identification, which provides an effective way of completely degrading chlorinated hydrocarbon pollutants in natural groundwater environment.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
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IF 7.864
Ruiyang Zhang,Tao Ran,Yuehan Cao,Qian Zhang,Fan Dong,Guidong Yang,Ying Zhou
Catalysis oxidization has been known to be an effective technique in environmental remediation. However, low efficiency for oxygen activation and difficult recovery of the catalysts in powdery form significantly limit the practical application. In this work, a new-type monolithic α-Ni(OH)2/Ni-foam was fabricated by the hydrothermal process. We found that H atoms of α-Ni(OH)2 can significantly promote oxygen activation, which endows it with favorable NO and NO2 oxidization confirmed by theoretical calculation and in situ DRIFTS. Furthermore, the introduction of Ni foam accelerated the pollutant gas transfer and charge carriers’ separation because of its abundant porous structure and high conductivity and its monolithic property simplified the recycling operation. Consequently, the obtained α-Ni(OH)2/Ni-foam achieved an excellent NO oxidation (69.0%) and no toxic NO2 was detected under visible light illumination (λ > 420 nm), indicating its highly promising potential in environmental remediation. Our work provides a conceptually different fresh perception to promote oxygen activation for highly efficient gas purification.
研究领域:
环境科学
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催化材料
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理论计算
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产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Wancheng Zhao,Jiapeng Ma,Dong Tian,Baotao Kang,Fangquan Xia,Jing Cheng,Yajun Wu,Mengyao Wang,Gang Wu
ABSTRACT In order to reduce energy consumption in water electrolysis, it is of great importance to design active and stable electrocatalysts for hydrogen evolution reaction (HER) in alkaline solution, especially based on earth-abundant metal. Here we integrate carbon nanotubes (CNTs) and Ni-Ni(OH) 2 heterostructure multifunctional components to design a self-supported 3D CNTs-Ni-Ni(OH) 2 catalyst for HER by composite deposition and subsequent in-situ oxidation . In alkaline solution, this designed CNTs-Ni-Ni(OH) 2 catalyst exhibits 0 mV onset overpotential, and overpotentials of 65 mV and 109 mV at 10 and 50 mA/cm 2 respectively. Electrochemical measurements, characterizations, and simulation results attribute the outstanding performance to the incorporation of CNTs and heterostructure . CNTs induce the formation 3D catalytic surface, enhance electrochemical active surface area , and more importantly weaken the adsorption of H. Moreover, the formation of heterostructure, especially reversible Ni(OH) 2 , supplies active sites and adjusts the adsorption strength of H atom to an optimal value. CNTs and heterostructure synergistically facilitate water adsorption, promote water dissociation, and accelerate H 2 desorption. Significantly, integration of multifunctional components supplies a distinct strategy for development of cost-effective electrocatalyst with outstanding performance.
研究领域:
材料科学
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电化学
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催化
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纳米技术
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DOI
高影响因子
DALTON TRANSACTIONS
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2023
·Vol. 52
·期 4
·928-935
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IF 4
Yidan Sun,Fang Liu,Xuerong Wang,Kangkang Lu,Xiaojing Liu,Yan Huang,Fengjiao Yu,Yuhui Chen
Efficient catalysts are highly desirable for the selective electrochemical CO2 reduction reaction (CO2RR). Ni single-atom catalysts are known as promising CO2RR catalysts, while Ni NPs are expected to catalyze the competing HER. In this work, we have modified the Ni NPs by encapsulating them into porous Ni–N–C nanosheets (Ni@Ni–N–C), to boost the synergy between Ni NPs and dispersed Ni–N species towards CO2RR. The CO faradaic efficiency (FECO) reached 96.4% at −0.9 V and retained over 90% in a wide potential window. More importantly, FECO values of over 94% have been obtained from −50 to −170 mA cm−2 with a peak FECO of 99% in a flow cell. Our work demonstrates that the surface modification of Ni NPs can inhibit the unexpected HER and activate the surface sites, offering a practical design strategy for CO2RR catalysts.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
Green Energy & Environment
·
2024
·
IF 10.7
Junming Zeng,Yongbin Yao,Fang Wang,Jiajian Gao,Lili Zhang,Guangwen Xu,Ziyi Zhong,Fabing Su
Nickle-based catalysts are commonly used for CO 2 methanation. However, there is still potential to improve their catalytic performance under mild conditions. In this study, we synthesized a series of Ru-Ni-Al catalysts from Ru-doped NiAl-hydrotalcite using a hydrothermal method. The Ru-Ni-Al catalyst demonstrated much higher activity for CO 2 methanation than the Ni-Al catalyst that did not have Ru doping. Both experimental results and theoretical calculations indicate that the enhanced performance of the Ru-Ni-Al catalyst is related to electronic interactions between nickel (Ni) and ruthenium (Ru). The Ru sites transfer electrons to the Ni sites, increasing the local electron density of Ni, which enhances the adsorption and activation of H 2 . Furthermore, the Ru-Ni metal interface sites improve the adsorption and activation of CO 2 . In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis indicates that adjusting the electronic structure of Ni sites can accelerate the production of intermediates HCOO*, while Ru-Ni intermetallic interface sites can directly dissociate CO 2 into CO*. In addition, CO 2 methanation on the Ru-Ni-Al catalyst follows HCOO*- and CO*-mediated pathways. This study underscores the potential for enhancing CO 2 methanation performance by modulating the electronic structure of Ni sites.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
FUEL
·
2019
·
IF 5.128
Xiaodong Li,Yanli Huang,Qian Zhang,Zhijun Zuo,Xiaodong Wang,Vladimir A. Vinokurov,Zheng Wang,Wei Huang
Ni-MoCeZr-MgAl(O) mixed oxide catalysts were successfully prepared from the Ce, Zr and Mo promoted hydrotalcite-like compounds (HTLcs) precursors using the simple and effective hexamethylenetetramine(HMT)-assisted hydrothermal synthesis method by tuning the molar ratio of n(HMT)/n(NO 3 − ). The influence of Ni content (3, 4.8, 6, 9 and 12%) on the catalytic performance of these catalysts in dry reforming of methane (DRM) was focused. Adjusting the content of Ni was able to change the metal dispersion and metal particle size, and small-sized (around 7 nm) and evenly dispersed Ni particles were obtained at Ni content of 6%. The catalyst with 6% Ni loading stood out for the high activity and stability, the CH 4 conversion of which fluctuated around 95% continuously for 610 h under GHSV of 60,000 mL·g cat −1 ·h −1 , and it was still above 92.8% throughout the 36-h-duration DRM experiments under GHSV of 80,000 mL·g cat −1 ·h −1 . This research may provide a simple and effective methodology for the synthesis of stable and efficient DRM catalysts.
研究领域:
催化化学
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材料科学
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能源化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Xiubo Xie,Ming Chen,Peng Liu,Jiaxiang Shang,Tong Liu
The Mg-5.0 wt%Ni-2.3 wt%V nanocomposite has been produced through reducing NiCl 2 with the Mg-V nanoparticles (NPs) prepared by hydrogen plasma metal reaction (HPMR) approach. The in situ formed Ni and V particles of about 15 nm uniformly decorate on the surface of Mg NPs. The Ni NPs transform into Mg 2 Ni while the V NPs remain unchanged after first hydrogen absorption and desorption cycle at 673 K. They show synergistic catalytic effects on the hydrogen storage properties of Mg-Ni-V nanocomposite. The nanocomposite can absorb 4.6 wt% H 2 within 30 min at 473 K and desorb 5.2 wt% H 2 within 10 min at 623 K. The activation energies of hydrogenation/dehydrogenation processes are decreased to 52.8 and 85.1 kJ per mol H 2 , lower than those of the Mg-5.4 wt%Ni nanocomposite of 63.2 and 89.3 kJ per mol H 2 . The enhanced hydrogen storage performances of the Mg-Ni-V nanocomposite are mainly attributed to the synergistic catalytic effects of the Mg 2 Ni and V catalysts, and the nanosize effect of Mg NPs on the decrease of the hydrogen diffusion distance.
研究领域:
材料科学
·
化学工程
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产品关联
DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Kuan Wang,Zhe Cao,Junlei Wang,Zhen-Hong He,Dan Wang,Rong-Rong Zhang,Weitao Wang,Yang Yang,Zhao-Tie Liu
The development of non-precious metal catalysts in heterogeneous catalytic processes is of great importance to the hydrogenation of quinolines for both theoretical and industrial applications. Herein, an effective non-precious metal catalyst, 58% Fe 4 Ni 6 Cu 5 /MCM-41, was developed to catalyze the hydrogenation of quinolines under the green and mild conditions, which can achieve 97.5% conversion and exceeding 98% selectivity to tetrahydroquinoline in solvent-free at low temperature of 50 °C. Moreover, the acceptable results of the reusability and gram scale-up experiments proved an industrial application potential of the as-prepared catalyst. Meanwhile, in cyclohexane system, 58% Fe 4 Ni 6 Cu 5 /MCM-41 catalyst can further realize a higher activity of the hydrogenation at a lower temperature of 40 °C, achieving 98.2% conversion and 98% selectivity to tetrahydroquinoline. The existence of Fe-Ni and Ni-Cu alloys in Fe 4 Ni 6 Cu 5 /MCM-41 catalyst was demonstrated by TEM, XRD, XPS, H 2 -TPD, and Raman spectroscopy. And, Fe-Ni and Ni-Cu alloys can be well dispersed onto MCM-41 molecular sieves. For Fe 4 Ni 6 Cu 5 /MCM-41 catalyst, quinoline molecules can be adsorbed by Fe 3+ species on the surface of Fe-Ni alloy through the coordination, while hydrogen molecules can be adsorbed and activated by Ni-Cu alloy. Under the synergism of Fe-Ni and Ni-Cu alloys, the highly effective and selective hydrogenation of quinolines was achieved at low temperature and in solvent-free system. The present approach offers a prospective idea for building non-precious metal catalysts to realize the effective hydrogenation of N-heterocyclic compounds under mild conditions.
研究领域:
催化化学
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材料科学
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绿色化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）