CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Bolong Jiang,Yuhan Zhang,Huan Wang,Kun Liu,Nan Jiang,Jiayou Li,Hua Song,Yanguang Chen
Hydrodeoxygenation (HDO) plays a crucial role in upgrading pyrolysis-oil derived from biomass. Here we describe a method for fabricating a carbon-encapsulated nickel metal–acid bifunctional catalyst (Ni@C/RCS-Al) supported on aluminum-doped radial channel silica (RCS-Al). This catalyst exhibits a large surface area and highly dispersed accessible active sites, achieved through a combination of salicylate- and MOF-assisted strategies. The RCS-Al was prepared by a one-pot salicylate-assisted hydrothermal method in an aqueous phase containing an Al source, which is simple, has a high yield, and saves time. The results show that Ni@C/RCS-Al displays a well-defined radial channel pore structure with a mesopore diameter of 31.1 nm, which can significantly increase the number of accessible active sites and accelerate mass transfer. The MOF-assisted strategy leads to the formation of highly dispersed smaller carbon-encapsulated nickel nanoparticle active sites, and Al doping contributes to the adjustable acid sites, demonstrating that Ni@C/RCS-Al is a metal–acid bifunctional catalyst. Importantly, the kinetics study revealed a high reaction constant for the constructed Ni@C/RCS-Al catalyst. Ni@C/RCS-Al demonstrates remarkable performance in HDO, achieving complete m -cresol conversion and 100 % selectivity to the target product methylcyclohexane within a brief period of 75 min (T = 250 °C p = 2 MPa, m-cresol/catalyst (g) = 7.5). This exceptional performance stems from its radial channel pore structure and optimization of metal–acid sites. The thin carbon layer on the Ni surface contributes to its superior stability and water resistance, as verified by an experimental study and DFT calculations. This work opens up a new idea for the application of radial channel silica-supported catalysts in various reactions.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
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IF 10.8
Yibing Xie,Xueqian Wang,Zan Qu,Ping Ning,Langlang Wang,Haomiao Xu,Wenjun Huang,Jichang Lu,Jianfei Luo
The transformation of toxic arsine (AsH3) gas into valuable elemental arsenic (As0) from industrial exhaust gases is important for achieving sustainable development goals. Although advanced arsenic removal catalysts can improve the removal efficiency of AsH3, toxic arsenic oxides generated during this process have not received adequate attention. In light of this, a novel approach for obtaining stable As0 products was proposed by performing controlled moderate oxidation. We designed a tailored Ni-based catalyst through an acid etching approach to alter interactions between Ni and NaY. As a result, the 1Ni/NaY-H catalyst yielded an unprecedented proportion of As0 as the major product (65%), which is superior to those of other reported catalysts that only produced arsenic oxides. Density functional theory calculations clarified that Ni species changed the electronic structure of oxygen atoms, and the formed [NiIII–OH (μ-O)] active centers facilitated the adsorption of AsH2*, AsH*, and As* reaction intermediates for As–H bond cleavage, thereby decreasing the direct reactivity of oxygen with the arsenic intermediates. This work presents pioneering insights into inhibiting excessive oxidation during AsH3 removal, demonstrating potential environmental applications for recovery of As0 from toxic AsH3.
研究领域:
环境科学
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催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ORGANOMETALLICS
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2022
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IF 3.837
Shu Jiang,Yuting Zheng,Ming Liu,Zhixin Yu,Yanping Ma,Gregory A. Solan,Wenjuan Zhang,Tongling Liang,Wen-Hua Sun
Ten examples of nickel(II) halide complexes [8-{N(2,4-(C15H13)2-6-RC6H2N)}C9H8N]NiBr2 [R = Me (Ni1), Et (Ni2), iPr (Ni3), Cl (Ni4), or F (Ni5)] and [8-{N(2,4-(C15H13)2-6-RC6H2N)}C9H8N]NiCl2 [R = Me (Ni6), Et (Ni7), iPr (Ni8), Cl (Ni9), or F (Ni10)], each incorporating a sterically encumbered N,N-chelating 8-[2,4-bis(dibenzocycloheptyl)-6-R-phenylimino]-5,6,7-trihydroquinoline ligand, are disclosed. Full details for the preparation of these complexes as well as the zinc-mediated synthesis of precursor ligands L1–L5 are given. Structural characterization of Ni3(H2O), Ni6, Ni7(H2O), and Ni8(H2O) reveals halide-bridged dinuclear structures of the type (N,N)NiX(μ-X)2NiX(N,N) with the ortho-substituted dibenzocycloheptyl groups providing steric protection to each metal center. In the presence of ethylaluminum dichloride (EtAlCl2) or methylaluminoxane (MAO), Ni1–Ni10 displayed high activities for ethylene polymerization [≤6.17 × 106 g of PE (mol of Ni)−1 h–1 for Ni6/EtAlCl2 at 20 °C], generating low-molecular weight polyethylene waxes. Notably, catalysts incorporating a 6-alkyl group (Me, Et, or iPr) as the N-aryl substituent proved to be more active than their 6-halide (Cl or F) counterparts and formed relatively higher-molecular weight polymers (Mw range of 9.1–22.9 kg mol–1) with a narrow dispersity. Moreover, analysis of these waxes by 13C nuclear magnetic resonance spectroscopy showed that they typically possessed short chain branching (>83% methyl) with branching densities of 79–90 branches per 1000 Cs. In addition, chain end analysis revealed the presence of both vinyl (−CH═CH2) and internal vinylene (−CH═CH−) functional groups, highlighting the role of both β-H elimination and isomerization.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
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2019
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IF 7.723
Kaikai Liu,Hongliang Xin,Minghan Han
The phosphorus (III) ligands were crucial for the further improvement of homogeneous nickel catalysts that were employed in the isomerization of 2-methyl-3-butenenitrile (2M3BN) to 3-pentenenitrile (3PN). The catalytic behavior of 1,4-bis(diphenylphosphino)butane (dppb 1 )Ni complex was improved in cumene and the conversion of 2M3BN showed zero-order kinetic. The mechanism behind the isomerization was amended and the density functional theory (DFT) calculations suggested that the reductive elimination step forming 3PN was kinetically relevant in catalytic cycles. An optimal bite angle of nickel-diphosphine complex around 104.7° provided excellent catalytic performance. The key factors governing isomerization were unraveled. The steric effect determined the reactivity, while the electronic effect governed the selectivity of the isomerization reaction. The bite angle – a vital descriptor – would associate with the steric and electronic effects of diphosphines. These structure-activity relationships provided important guidance for ligand design in the isomerization of 2M3BN.
研究领域:
化学
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催化科学
✓ 已验证
DOI
高影响因子
CATALYSIS TODAY
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2020
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IF 5.825
Hong Du,Xiuyun Ma,Miao Jiang,Peifang Yan,Yang Zhao,Z. Conrad Zhang
The lignocellulosic biomass utilization is a feasible way to obtain alternative fuels and chemicals. Xylitol as an ideal sweetener is one of the top twelve value-added chemicals derived from biomass. Xylitol is also used in the pharmaceutical and cosmetics industries. Thus, the production of xylitol from biomass is significantly important. A silica supported nickel catalyst derived from nickel phyllosilicate for efficient aqueous phase xylose hydrogenation to xylitol was developed in this study. Higher xylose conversion was observed over the nickel phyllosilicate derived catalyst compared to nickel oxide derived nickel catalyst prepared by impregnation and commercial Raney Ni catalyst. The excellent xylitol selectivity (approximately 99 %) was also obtained over the nickel phyllosilicate derived catalyst. The differences in structure and property resulted from different preparation methods were investigated by means of XRF, N 2 physisorption, XRD, FT-IR, H 2 -TPR, TEM as well as H 2 -TPD. The higher nickel dispersion of nickel phyllosilicate derived catalysts, which could be synthesized by ammonia evaporation and deposition-precipitation using Na 2 CO 3 as precipitator, led to higher xylose conversion. In addition, the phyllosilicate derived nickel catalyst demonstrated outstanding stability. Consequently, phyllosilicate derived nickel catalyst is promising for the industrial application for the production of xylitol form xylose aqueous hydrogenation thanks to its higher activity and selectivity as well as good stability.
研究领域:
化学工程
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催化材料
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
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2012
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IF 2.721
Hualiang Zuo,Qiying Liu,Tiejun Wang,Longlong Ma,Qi Zhang,Qing Zhang
Catalytic hydrodeoxygenation (HDO) of vegetable oils to renewable alkane-type biofuels has attracted more and more concern in recent years. However, the presently used catalysts were mainly focused on the sulfided CoMo and NiMo catalysts, which inevitably posed sulfur contamination in final products. Therefore, exploring nonsulfured catalyst for this processing is of fundamental importance, but it is still an open challenge. In this paper, we prepared the sulfur free Ni supported on SiO2, γ-Al2O3, SAPO-11, HZSM-5, and HY by incipient wetness impregnation and tested the catalytic performance in HDO of methyl palmitate. Alkanes with long carbon chains were mainly produced with two possibly parallel approaches: hydrogenation of hexadecanal to hexadecanol, followed by dehydration/hydrogenation to C16 alkane and decarbonylaton/decarboxylation of hexadecanoic acid to C15 alkane. The acidity of catalysts significantly influenced their catalytic performance, and the Ni/SAPO-11 catalysts with weak and medium acidity showed superior properties to the other catalysts due to the synergistic effect of metal Ni and acidic support. The maximum yield of 93% for C15+ alkanes was observed over 7 wt % Ni/SAPO-11 under the mild reaction conditions of 493 K and 2 MPa, indicating its promising application in this reaction.
研究领域:
催化化学
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可再生能源
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2024
·Vol. 14
·期 23
·6814-6823
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IF 4.4
Xihui Yang,Zekun Li,Zikun Yang,Dapeng Meng,Zhao Wang
The development of efficient and stable bifunctional non-noble metal catalysts for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is essential for electrochemical water splitting. In this study, CoNi@C core–shell structure catalysts derived from ZIF-67 were synthesized through high-temperature calcination. The hydrophilic carbon shell inhibits the oxidation of Co and Ni and enhances the activity and stability of the water splitting reaction. CoNi serves as the active site of the reaction, while the doped nitrogen further promotes the electrocatalytic reaction. The synthesized Ni1Co10/C catalyst exhibits high bifunctional performance, with low overpotentials at 100 mA cm−2 for the OER (380 mV) and HER (357 mV), and a high double-layer capacitance (54 mF cm−2). Moreover, the Ni1Co10/C catalyst serves as an effective cathode for water splitting in a two-electrode system, demonstrating a stable cell voltage of 2.05 V and maintaining a constant catalytic current of 100 mA cm−2 over 24 hours. DFT calculation showed that the active site of the OER and HER was Co.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2025
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IF 4.1
Zongze Li,Kedi Yu,Yumin Leng,Zhengbo Chen
The direct methanol fuel cells (DMFCs) stand out among various types of fuel cells due to their advantages of pollution-free operation, rational design, and high energy density. However, the development of methanol fuel cells faces several obstacles. Platinum-based catalysts are considered the most promising type of catalyst for electrochemical methanol oxidation reaction (MOR), yet they are limited by issues inherent to commercial platinum–carbon (Pt/C) catalysts, including high platinum content, low activity, rapid deactivation, and susceptibility to poisoning, all of which restrict their practical applications in methanol oxidation cells. Based on the platinum-based metal system, this study explores a platinum-nickel (PtNi) bimetallic nanomaterial with a nanowire microstructure as an alternative catalyst for MOR. The PtNi nanowires possess more active sites and exhibit synergistic effects, thereby enhancing catalytic performance.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2025
·
IF 4
Fuzeyu Zhong,Weixiao Sun,Xiaohu Ge,Keng Sang,Huihui Qian,Wenyao Chen,Gang Qian,Yueqiang Cao,Jianrong Zeng,Lina Li,Xuezhi Duan,Xinggui Zhou,Jing Zhang
Catalytic hydrogenative rearrangement of furanic aldehydes is crucial for producing biomass-derived cyclopentanone fine chemicals. However, designing highly selective catalysts remains challenging due to the interplay among tandem hydrogenation, ring-opening, aldol condensation, dehydration, and parallel ring-hydrogenation. Here, we employ a single self-assembly step by depositing phosphonic acids (PAs) on conventional Ni catalysts to introduce tunable interfacial Brønsted acid sites (BAS), resulting in an unprecedented 3-hydroxymethyl-cyclopentanone yield of 95.8% from hydroxymethylfurfural. Kinetic studies reveal a one-order-of-magnitude increase in ring-opening rates—the slow step in hydrogenative rearrangement—after PAs modification, accompanied by a drop in the apparent activation energy from 154.1 to 105.4 kJ mol −1 . In contrast, the activation energy for the ring-hydrogenation side reaction remains almost unchanged. Theoretical calculations suggest that BAS synergize with adjacent Ni to lower the C–O cleavage barrier by providing protons to attack the hydroxymethyl oxygen atom, which is the key step to initiate ring-opening.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Xinyu Liu,Xixi Meng,Tao Zhong,Yuxin Wang,Fuying Wu,Hu Liu,Hong Li,Liuting Zhang
Magnesium hydride (MgH 2 ) with its high hydrogen storage capacity (7.6 wt%) and exceptional reversibility, has emerged as a promising solid-state hydrogen storage material. This study designed a polymeric carbon nitride (PCN) supported single-phase Ni catalyst with superior thermal stability and catalytic activity. The optimized PCN-Ni catalyst significantly reduced the initial dehydrogenation temperature of MgH 2 to 192 ºC. At 295 ºC, the composite released 6.10 wt% H 2 within 5 min, and it subsequently absorbed 5.50 wt% H 2 within 5 min at 150 ºC. Compared to pristine MgH 2 , the activation energies for dehydrogenation and hydrogen absorption were reduced by 31.6 % and 29.4 %, respectively. Moreover, the MgH 2 + 10 wt% PCN-Ni composite exhibited remarkable cycling stability, with capacity retention rates of 96.0 % and 96.7 % after 20 hydrogenation/dehydrogenation cycles. In conclusion, this work provides a new perspective on the heterogeneous synergy of transition metal and carbon nitride composite catalysts in promoting the dehydrogenation/rehydrogenation reactions of MgH 2 and lays the foundation for the design and fabrication of highly efficient catalysts in other energy storage related fields.
研究领域:
材料科学
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能源存储
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Precision Chemistry
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2023
·
IF 0
Yating Lv,Hai Wang,Huixin Wu,Qingsong Luo,Liang Wang,Feng-Shou Xiao
Selective hydrogenation over earth-abundant metal catalysts is challenging but particularly valuable for practical applications in heterogeneous catalysis. Herein, we demonstrate that the catalytic selectivity of the commercial Raney nickel catalyst can be greatly tuned by modulation of the nickel surface by silica. Using quinoline hydrogenation as a model, we show that the silica-modified Raney nickel catalysts exhibit good activity, excellent selectivity, and long stability, whereas the undesired overhydrogenation reactions are effectively hindered. In contrast, the pristine Raney nickel catalyst shows inferior selectivity for the targeted product. Mechanistic studies confirm a positive role of silica to facilitate the desorption of 1,2,3,4-tetrahydroquinoline from the catalyst surface, thus enhancing the product selectivity.
研究领域:
物理化学
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材料科学
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催化化学
✓ 已验证
DOI
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Ze-Wei Wu,Jing Xiong,Cun-Wen Wang,Yuan-Hang Qin
Although supported Ni is generally considered the most active non-noble metal catalyst for decomposing NH 3 to produce CO x -free H 2 , its activity is not sufficient. Herein, supporting high-loading Ni on SBA-15 is explored to alleviate the low intrinsic activity issue of Ni. SBA-15 supports with tunable textual properties are synthesized to support Ni catalyst for NH 3 decomposition. Characterization shows that Ni catalyst with a loading close to 40 wt% supported on SBA-15 with the largest specific surface area (Ni/SBA-15-80) exhibits a NH 3 decomposition performance much better than those reported on other Ni-based NH 3 decomposition catalysts, resulting from its favorable textural properties and high Ni loading. In addition, Ni/SBA-15-80 shows excellent catalytic stability, with no activity degradation over an 80-h NH 3 decomposition test. This work reveals the importance of textural properties of support and Ni loading to NH 3 decomposition performance and can provide a new idea for synthesizing high-performance NH 3 decomposition catalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
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