GREEN CHEMISTRY
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2024
·
IF 9.3
Shan Jiang,Riyang Shu,Anqi Wang,Zhuoli Deng,Yuhong Xiao,Jiajin Li,Qingwei Meng,Qian Zhang
High-quality liquid biofuels can be produced from renewable lignin-derived phenolic compounds through the efficient hydrodeoxygenation (HDO) process, in which the traditional catalysts usually include metal site and acid site that catalyzes hydrogenation and deoxygenation procedures respectively. This work presented a novel acid-free NixMoyN/C catalyst from the perspective of green chemistry, providing a new pathway for HDO of lignin-derived phenolic compounds that involves hydrogenation, deoxygenation and hydrogenolysis at the same time. A series of NixMoyN/C catalysts were prepared by varying Ni and Mo molar ratio, where the Ni1Mo3N/C catalyst showed the best HDO performance. Guaiacol was completely converted at 260 °C after 4 h, with 95.8% cyclohexane selectivity. And a small amount of benzene can be obtained as a valuable fuel additive by-product by altering the conventional HDO reaction path. By shortening the reaction time, benzene can be obtained as the intermediate products with a relative high selectivity. Based on the characterizations of XRD, BET, SEM, TEM, XPS, H2-TPD and EPR, the results demonstrate that the multiple active components of Ni1Mo3N/C catalyst allow it to efficiently catalyze the hydrogen activation and C-O bond cleavage even under acid-free condition. The existence of the active phase of Ni, Ni2Mo3N and β-Mo2C, as well as the interaction between Ni and Mo metals, contributes together to achieve an efficient HDO performance. Not only for the various phenolic model compounds, the feasibility of Ni1Mo3N/C catalysts for upgrading raw lignin-oil was also demonstrated, with the hydrocarbon content increasing from 5.7% to 88.4%. Notably, arenes account for 18.2% in the hydrocarbon products, which confirms the occurrence of hydrogenolysis in the catalytic process. This work provides a novel route for the conversion of lignin-derived phenolic compounds to the production of high-quality hydrocarbon liquid biofuels, especially the direct production of arene component.
研究领域:
化学工程
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催化
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可再生能源
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绿色化学
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Yanbin Qi,Yihua Zhu,Hongliang Jiang,Chunzhong Li
Designing efficient, stable, and easily scaled-up catalysts for nucleophile oxidation reactions (NOR) is a key step in promoting the industrial application of NOR. Here, a simple physical mixing strategy is adopted to prepare a mixture of NiMo oxide and CoMo oxide as catalyst for methanol electrocatalytic oxidation reaction (MOR). The mixture exhibits high catalytic activity for MOR and its performance far exceeds that of a single component. The interaction at the contact interface between nickel and cobalt components is clarified through operando electrochemical impedance spectroscopy, in-situ Raman spectroscopy, and a series of electrochemical tests. The interfacial interaction enhances the charge transport and promotes the formation of electrophilic OH* species, which significantly boosts the methanol oxidation reaction. This work provides a new idea for the design of efficient and easily scaled-up catalysts for nucleophile oxidation reactions.
研究领域:
催化
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电化学
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材料科学
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可持续能源
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Min Sun,Qing Ye,Lu Lin,Yufeng Wang,Zongmin Zheng,Fangfang Chen,Yongliang Cheng
Developing a high-efficiency hydrogen evolution reaction (HER) electrocatalyst for the large-scale production of hydrogen is essential but challenging. In this study, we used NiMo solid-solution alloy porous nanofibers to develop a robust HER electrocatalyst through electrospinning, oxidization, and high-temperature reduction treatment. In 1 M KOH electrolyte, the fabricated NiMo solid-solution alloy porous nanofibers exhibited higher HER activity than Ni nanofibers, which required a low overpotential of 69, 208, and 300 mV at 100, 500, and 1000 mA cm −2 , respectively, and had outstanding durability at 100 mA cm −2 over 60 h. We developed a promising candidate for a high-efficiency HER electrocatalyst, and our findings provided valuable information for fabricating highly robust alloy-based electrocatalysts.
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高影响因子
Catalysts
·
2019
·Vol. 9
·期 7
·596
·
IF 3.444
Ying Liu,Huan Zhang,Cong Ma,Nan Sun
Precious metal-free NiMoM (M = Pr2O3, Cu2O) catalysts have been synthesized through a simple coreduction method, without any surfactant or support material, and characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The resultant Pr2O3- or Cu2O-modified NiMo catalysts exhibit different structures, which is due to a difference in the synergistic effects of NiMo and the modifying elements. NiMoPr2O3has an amorphous structure, with low crystallinity and uniform particle dispersion, while NiMo@Cu2O adopts the core–shell structure, where the core and shell are synergistic with each other to promote electron transfer efficiency. The support material-free nanocatalysts Ni9Mo1(Pr2O3)0.375and Ni4Mo@Cu2O are both highly efficient compared with bimetallic NiMo catalysts, in terms of hydrogen generation from hydrous hydrazine (N2H4·H2O) at 343 K, with total turnover frequencies (TOFs) of 62 h−1and 71.4 h−1, respectively. Their corresponding activation energies (Ea) were determined to be 43.24 kJ mol−1and 46.47 kJ mol−1, respectively. This is the first report on the use of Pr-modified NiMo and core–shell NiMo@Cu2O catalysts, and these results may be used to promote the effective application of noble metal-free nanocatalysts for hydrogen production from hydrous hydrazine.Keywords:NiMoM (M = Pr2O3, Cu2O) catalysts;hydrous hydrazine;hydrogen production
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Catalysts
·
2025
·Vol. 16
·期 1
·
IF 4
Haidong Li,Mingjia Liu,Yifang Zhang,Xiu Chen,Kunyi Zheng,Xilong Wang,Penglei Ni,Jun Ma
The selective hydrocracking of polycyclic aromatic hydrocarbons to BTX requires precise control over catalyst porosity and metal–acid balance. Hierarchical porosity, integrating microporous and mesoporous networks, is pivotal for enhancing mass transport and regulating reaction pathways. USY zeolites were engineered to create distinct hierarchical architectures via HCl, urea, and NaOH–surfactant treatments. HCl treatment constructed a gradient pore acidity system, urea treatment enhanced acidity while preserving microporosity, and NaOH–surfactant fabricated ordered mesopores with reduced acidity. The catalyst with the HCl-engineered gradient pore (NiMo/YH-1) achieved a 91% BTX yield at 425 °C in naphthalene hydrocracking, outperforming others. This performance is attributed to its gradient structure that enforces an optimal “hydrogenation-then-cracking” pathway, highlighting the critical role of tailored hierarchical porosity.
研究领域:
催化化学
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石油化工
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材料科学
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化学反应工程
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Jia-Yi Chen,Yu-Shu Han,Qing He,Yu-Qiong Huang,Ju-Hua Li,Zhong-Li Wang
A strong interaction interface is constructed between TiO 2 particles and NiMo nanorods. • NiMo alloy electrodes with and without TiO 2 exhibit different reconstruction processes as both anode and cathode. • TiO 2 tailored NiMo electrodes exhibits excellent activity and stability for over 10,000 h at 500 mA cm −2 in 30% KOH at 80 °C. • The reaction mechanism was systematically studied by in situ Raman spectroscopy and 18 O isotope labeling. The reconstruction process of electrocatalysts plays an important role in the electrocatalytic process, and how to tailor the reconstruction is crucial for the performance and remains greatly challenging. Herein, we demonstrate that TiO 2 can tailor the reconstruction process of NiMo alloy for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) reactions. NiMoO 4 microrods arrays adsorbed with titanium butoxide on its surface are converted into TiO 2 modified NiMo alloy under high-temperature reduction. NiMo alloy electrodes with and without TiO 2 exhibit different reconstruction processes as both anode and cathode under simulated industrial conditions (30% KOH, 80 °C). With TiO 2 , the cathode and anode are reconstructed into ultrafine Ni(OH) 2 nanosheets coated on NiMo alloy and ultrafine NiOOH nanosheets, respectively. Without TiO 2 , NiMo alloy electrodes are reconstructed into large-sized Ni(OH) 2 or NiOOH nanosheets on the cathode or anode. The TiO 2 tailored NiMo electrodes exhibit low overpotentials of 29 mV for HER and 213 mV for OER at a current density of 10 mA cm −2 in 1 M KOH at 25 °C. Moreover, an electrolytic cell assembled by them as both cathode and anode electrodes can maintain 1.8 V at a current density 500 mA cm −2 with stable running for over 10,000 h in 30% KOH at 80 °C. Mechanism studies indicate that TiO 3 2− ions intercalate into the interlayer of Ni(OH) 2 , inhibiting the dissolution of Mo and controlling the size of Ni(OH) 2 , and the bond lengths of Ni O and Ni Mo bonds are shortened, which effectively enhance catalytic activity and stability. Download: Download high-res image (60KB) Download: Download full-size image
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Yunfang Yan,Xuejie Cao,Liangmin Ning,Fei Lin,Wenzhuo Qin,Xin Liu,Wen Gu
The construction of low-cost electrocatalysts with good conductivity, excellent intrinsic activity, and superior stability is crucial for the hydrogen evolution reaction (HER). Herein, we report an outstanding catalyst (Ni0.2Mo0.8N/NiMoP2/MoO2@NC) consisting of NiMo-based nanorod arrays supported on Ni foams for the efficient alkaline HER. It shows an ultralow overpotential of 48 mV and remarkable longevity for over 145 h at 10 mA cm–2 in 1.0 M KOH. The integration of ample compositions is favorable to the formation of heterointerfaces, accelerating electron transfer. The assembly of transition metal nitrides and phosphides fully develops the electrical conductivity of metal materials, which paves the way for superstability. The superior electrocatalytic activities can be attributed to the vital features, including the synergistic effect of Ni0.2Mo0.8N and NiMoP2, good electrical conductivity of MoO2, and corrosion resistance of NC basement. The present work proposes that regulating compositions and hierarchical nanostructures are of significance in developing electrode materials for the HER.
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高影响因子
Catalysts
·
2022
·Vol. 12
·期 4
·371
·
IF 4.501
Minghao Zhou,Fei Ge,Jing Li,Haihong Xia,Junli Liu,Jianchun Jiang,Changzhou Chen,Jun Zhao,Xiaohui Yang
Lignin is an attractive renewable source of aromatics with a low effective hydrogen to carbon ratio (H/Ceff). The catalytic hydrodeoxygenation (HDO) of lignin-derived model compounds is a key strategy for lignin upgrading. In this work, the HDO of guaiacol, a typical lignin-derived compound, was carried out over metal–organic framework (MOF)-derived Ni-based catalysts. A monometallic Ni-MOF catalyst and different ratios of bimetallic NiMo-MOF catalysts were synthesized by a hydrothermal process, followed by a carbonization process. Among these catalysts, Ni3Mo1@C exhibited an excellent catalytic performance, affording a guaiacol conversion of 98.8% and a cyclohexanol selectivity of 66.8% at 240 °C and 2 MPa H2for 4 h. The addition of Mo decreased the particle size of the spherical structure and improved the dispersion of metal particles. The synergistic effect between Ni and Mo was confirmed by various means, including ICP, XRD, SEM, TEM, and NH3-TPD analyses. In addition, the effect of the reaction temperature, time, and H2pressure during the HDO process is discussed in detail.Keywords:guaiacol;hydrodeoxygenation;Ni-based bimetallic catalysts;MOF
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高影响因子
CRYSTENGCOMM
·
2024
·
IF 2.6
Guixin Zhao,Sixuan Zhang,Jinzhao Huang,Zehui Liu,Feng Jiao,Ke Zhang,Yu Zhang,Xiaolong Deng
NiMo-based polyalloy catalyst is a non-precious metal-based high-entropy alloy catalyst that has been extensively studied in recent years. It exhibits superior electrochemical performance in electrocatalytic water splitting for hydrogen production, and the combination of NiMo-based polyalloy catalysts with carbon black substrates is expected to produce better electrochemical supports. In this paper, we prepared a series of carbon-based high-entropy heterogeneous material catalysts using zero-dimensional carbon black, one-dimensional carbon nanotubes and two-dimensional graphene as substrates, respectively. Analytical results through structural characterization of the synthesized materials as well as electrochemical tests revealed that carbon black, which is in the form of nanoparticles, can be more tightly wrapped with Ni shells compared to tubular nanotubes and flake graphene, which can effectively increase the number of active sites, thus promoting the outstanding performance of the zero-dimensional carbon-based transition metal nanomaterial catalysts NiMoCoMnLa/CB@Ni in alkaline electrocatalytic hydrogen precipitation reaction . Driven by these findings, this work may provide new ideas in the pathway of rationally designing zero-dimensional carbon-based high-entropy alloy nanoparticle catalysts as efficient electrocatalysts in green hydrogen production processes.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Chemistry-An Asian Journal
·
2026
·Vol. 21
·期 6
·e70687
·
IF 3.2
Chuanxiang Zhang,Mingyue Zhang,Hao Zhang,Zhixin Liu,Xingxu Gao,Jianping He
This study used a one-step electrodeposition method to grow nickel molybdenum alloy catalysts (NiMo/NM) with both crystalline and amorphous states on a Ni mesh substrate. x-ray diffraction (XRD) and x-ray photoelectron spectroscopy (XPS) jointly confirmed that the insertion of Mo atoms into the Ni lattice resulted in a heterogeneous interface with the coexistence of crystalline and amorphous states. The scanning electron microscopy (SEM) test results show that the surface of NiMo/NM alloy owns a “cauliflower-like” morphology, which increases the specific surface area of the catalyst and exposes more catalytic active sites. Under the combined action of NiMo heterogeneous interface and highly rough surface on the catalyst surface, the catalyst exhibits superior hydrogen evolution reduction (HER) catalytic activity and long-term operational stability in alkaline solutions compared to commercial catalysts Pt/C. Especially under high current densities in industrial applications and conditions simulating alkaline seawater electrolytes, NiMo/NM exhibits catalytic stability in hydrogen evolution due to the stability of its NiMo alloy structure.
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Wenbin Wang,Wei Yang,Xin Yu,Tao Long,Sha Deng,Qiya Bian,Qingyun Ji,Yunlong Guo
Developing efficient electrochemical hydrogen evolution reactions (HER) and nitrate reduction reactions (NitRR) is of great significance for alleviating the growing energy demand and environmental pollution. In this study, Te–Cu 2 O/NiMo electrocatalyst with nanospheres structure was successfully synthesized on foam nickel molybdenum substrate by electrodeposition, and its performance in electrochemical hydrogen evolution reaction (HER) and nitrate reduction reaction (NitRR) was further evaluated. In a 1.0 M KOH solution, the Te–Cu 2 O/NiMo catalyst exhibits good catalytic activity at a current density of 10 mA cm −2 , with an overpotential of 140.67 mV and a Tafel slope of 136.72 mV dec −1 . Further testing showed that at current densities above 120 mA cm −2 , the performance of the catalyst even surpassed that of commercial Pt/C. In addition, Te–Cu 2 O/NiMo exhibits good stability during electrolysis that is up to 60 h. During the nitrate reduction process, the catalyst increased the nitrate removal rate to 65 % within 180 min of constant current electrolysis, while achieving a NH 4 + - N conversion efficiency of 59.1 %, with almost negligible NO 2 − - N generation. In summary, Te–Cu 2 O/NiMo catalyst exhibits dual functional advantages in HER and NitRR, providing new ideas and application prospects for the development of efficient electrocatalysts.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Ya Liu,Wenzhu Tang,Gaowei Zhang,Wenhao Chen,Qingze Chen,Chunlin Xiao,Shenghui Xie,Yejun Qiu
Developing stable and efficient electrocatalysts for hydrogen evolution reaction is of great significance for the production of clean hydrogen energy from water splitting. In this work, 3D AgNWs@NiMo/PU electrode was obtained by electrodepositing NiMo alloy onto three-dimensional silver nanowires conductive substrate (3D AgNWs/PU) which was uniformly assembled on the surface of the skeleton of a polyurethane sponge (PU). 3D AgNWs/PU provides good electrolyte permeability, rich active site attachment points, good electronic conductivity and electrocatalytic synergy, which greatly improves the catalytic activity. In addition, 3D AgNWs@NiMo/PU electrode does not need to use adhesive in the process of hydrogen evolution, which can improve the hydrogen evolution performance and stability of the electrode. Specifically, the optimized electrode (AgNWs@NiMo/PU-1200 s) exhibits excellent hydrogen evolution performance by achieving a low overpotential of 32 mV (vs. RHE) at a current density of 10 mA cm −2 , with a Tafel slope of 72 mV dec -1 (in 1 M KOH). More interestingly, it also has good stability after 10 h of stability test. Therefore, this study provides a feasible way to develop stable and efficient 3D HER electrocatalysts.
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