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Molecular Catalysis · 2017 · IF 0

Highly selective liquid-phase hydrogenation of furfural over N-doped carbon supported metallic nickel catalyst under mild conditions

Wanbing Gong,Chun Chen,Haimin Zhang,Yong Zhang,Yunxia Zhang,Guozhong Wang,Huijun Zhao

In this work, N-doped activated carbon supported metallic nickel (Ni/NAC) catalysts were fabricated by two-step calcination method in N 2 atmosphere for liquid-phase hydrogenation of furfural (FAL). It was found that the pyrolysis temperature and amount of melamine as N doping source have important influence on N doping content and type in activated carbon (AC) support, resulting in the subsequently formed Ni nanoparticles on N-doped AC with different sizes and thus affording different catalytic hydrogenation activities. The results demonstrated that using N-doped AC with 1.0   g melamine at 1073   K in N 2 atmosphere as support, the obtained Ni/NAC at 873   K in N 2 atmosphere with Ni nanoparticle sizes of ∼13.1   nm (denoted as Ni/NAC-1-1073) exhibits a N doping content of 3.65   at.% and a surface area of 561.2   m 2   g −1 with a microporous structure. As catalyst for FAL hydrogenation, Ni/NAC-1-1073 demonstrated the best catalytic performance among all investigated catalysts, achieving almost 100% selectivity of tetrahydrofurfuryl alcohol (THFOL) with a complete FAL conversion at 353   K after 3   h reaction, while only 76.7% selectivity of THFOL with a FAL conversion of 86.4% was obtained using Ni/AC catalyst without N doping under the identical experimental conditions. Furthermore, it was found that almost 100% conversion of FAL to furfural alcohol (FOL) can be reached by transfer hydrogenation pathway in 2-proponal solvent using Ni/NAC-1-1073 at 413   K after 5   h reaction, whereas Ni/AC without N doping can only afford 30.2% conversion of FAL to FOL under the same conditions. The superior catalytic performance of Ni/NAC-1-1073 could be ascribed to a synergistic effect of nanosized Ni providing catalytic active sites, suitable N doping content and type in AC to promote catalytic performance, and advantageous structure characteristics of high surface area and porous structure favourable for the exposure of catalytic active sites and mass transport.

CAS / MDL: 7440-44-0 64365-11-3
研究领域: 催化化学 · 材料科学 · 可再生能源
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Selective hydrogenation of furfural over supported nickel and nickel phosphide catalysts

Qiumei Hou,Jingxuan Cai,Li Zuo,Hui Chen,Yuchuan Fu,Jianyi Shen

Supported Ni (60 wt% Ni) catalysts were prepared and phosphided into corresponding Ni 2 P catalysts. They were used for the hydrogenation of furfural as well as for the probe reactions (the hydrogenation of furan and propanal). The results demonstrated that the acidic support promoted the adsorption and hydrogenation of furan ring and aldehyde group over the nickel sites while the basic support played the opposite role. The IR spectra demonstrated that the aldehyde group was more easily hydrogenated than the furan ring at room temperature, implying the sequential hydrogenation of furfural to furfuryl alcohol (FA) and then to tetrahydrofurfuryl alcohol (THFA) over Ni. The microcalorimetric studies revealed that both the aldehyde group and furan ring were strongly adsorbed on Ni so that the Ni catalysts were highly active to hydrogenate the two groups, i.e., the Ni catalysts favored the formation of THFA. On the other side, although the adsorption heats of aldehyde group were much lower on Ni 2 P than on Ni, the adsorption heats were significantly higher for aldehyde group than for furan ring on Ni 2 P, implying the high selectivity to FA on Ni 2 P.

CAS / MDL: 142-82-5 603-35-0
研究领域: 催化化学 · 材料科学
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ACS Catalysis · 2022 · IF 13.7

Lattice Oxygen-Induced d-Band Shifting for Enhanced Hydrogen Oxidation Reaction on Nickel

Chang Sun,Pengcheng Zhao,Yongqing Yang,Zhuo Li,Wenchao Sheng

The application of anion exchange membrane fuel cells is hampered by the development of highly efficient and earth-abundant anode hydrogen oxidation reaction (HOR) catalysts. Here, a series of nickel catalysts (denoted as Ni-X) with different lattice oxygen (LO) contents were synthesized by H2 reduction of nickel hydroxide at temperatures (X) ranging from 300 to 500 °C. The Ni-400 (LO/Ni = 0.41, NiO0.41) catalyst with an optimum LO content showed excellent HOR activity and stability, comparable to current Ni-based electrocatalysts. An X-ray photoemission spectroscopic study, combined with density functional theory calculations, suggested that introducing LO into Ni modified the metal d-band electronic structure and in turn the hydrogen binding energy, which played a major role in determining the HOR performance.

CAS / MDL: 107-21-1
研究领域: 材料科学 · 电化学
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CHEMISTRY-A EUROPEAN JOURNAL · 2025 · IF 3.7

Ni(OH)x/Ni-Catalyzed In Situ Hydrogenation and Ethanol Ethoxylation of 2-Methylfuran for Renewable Biofuel Co-Upgrading

Jun Shen,Changhui Liang,Yuxin Zhang,Xiaoqiang Zhang,Huixiang Li,Yongxin Li,Songhai Xie,Z. Conrad Zhang

Bioethanol and furanics are currently prevailing additives to fossil-based transportation fuels. With the objective to lift the longstanding limitations of these biofuel additives, this work reports for the first time the synthesis of 2-ethoxy-2-methyltetrahydrofuran (2-EO-2-MTHF) as a co-upgraded fuel by reacting ethanol with 2-methylfuran (2-MF). The formation of 2-EO-2-MTHF is achieved through ethanol ethoxylation of 2-MF, enabled by a reverse Ni(OH) x /Ni catalyst under hydrogen pressure. Nickel hydroxide species over the Ni nanoparticles play a crucial role in activating ethanol and polarizing the partially hydrogenated dihydrofuran intermediates, favorably steering the reaction selectively toward the ethoxylation product. The reaction conditions, including pressure and temperature, are systematically optimized to enhance the yield of 2-EO-2-MTHF, and provide a means to beneficially tune the fuel compositions consisting mainly of 2-EO-2-MTHF and 2-MTHF, both are high energy density molecules. Importantly, the reverse Ni(OH) x -Ni catalyst allows a one-pot process to accomplish consecutive partial hydrogenation of 2-MF and ethanol ethoxylation. This work provides a practical strategy for upgrading biomass-derived polar primary fuel molecules into more versatile fuels and chemicals.

CAS / MDL: 7440-02-0 7791-20-0
研究领域: 化学工程 · 可再生能源 · 催化化学
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Catalysis Science & Technology · 2025 · IF 4.2

Efficient upgrading of polystyrene plastics to nitriles through a catalytic oxidative amination process

Chengyang Sun,Yong Guo,Xiaohui Liu,Yanqin Wang

The upcycling of C–C bond linked polyolefins has drawn wide attention in recent years and a lot of studies have been focused on the conversion of polyolefins to hydrocarbons, while the further valorization to more value-added products has barely been developed. In this work, we developed an efficient strategy to upgrade polystyrene (PS) plastics into a single N-containing product, benzonitrile, over a NiO/CeO2 catalyst via a one-pot, two-step process. The first step is the oxidative-amination of PS to a mixture of benzamide and benzonitrile and the second step is the dehydration of benzamide to benzonitrile; finally, a single N-containing product, benzonitrile with a 50.3% yield, was achieved. Mechanism studies via control experiments in the first oxidative-amination step showed that benzaldehyde was the important intermediate, which can undergo two parallel pathways generating benzamide and benzonitrile, respectively. Following the dehydration of benzamide to benzonitrile in the second step, benzonitrile was produced as the only product. This strategy can also be extended to real-life PS plastics and a high yield of benzonitrile was achieved. This novel study provides an efficient approach for upgrading waste plastics to a single high-value product.

CAS / MDL: 1306-38-3
研究领域: 化学工程 · 环境科学 · 催化科学
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JOURNAL OF HAZARDOUS MATERIALS · 2020 · IF 9.038

Rapid leaching and recovery of valuable metals from spent Lithium Ion batteries (LIBs) via environmentally benign subcritical nickel-containing water over chlorinated polyvinyl chloride

Theoneste Nshizirungu,Masud Rana,Young-Tae Jo,Jeong-Hun Park

This study presents the development of an effective and environmentally friendly method to leach and to recover valuable metals, such as lithium (Li) and cobalt (Co) from the spent lithium-ion batteries (LIBs) using subcritical water assisted by nickel catalyst and waste chlorinated polyvinyl chloride (CPVC). The effects of reaction parameters, such as Ni 2+ concentration, temperature, time, and liquid-solid ratio on the leaching efficiencies of Li and Co were carefully investigated. The solid residues obtained thereof were characterized by XRD and SEM-EDS analyses, while the leachates were analyzed by ICP-OES. The ICP-OES results showed that about 99.05% of Li and 98.08% of Co were effectively leached from the spent LiCoO 2 powder under the following optimized reaction conditions: temperature of 240 °C, reaction time of 40 min, Ni 2+ concentration of 0.04 M, and the liquid-solid ratio of 25:1 mL/g, respectively. Finally, based on the precipitation method, the Li and Co were recovered from the leachate as Li 2 CO 3 and Co(OH) 2 . The results and the method applied in this research suggest that the leaching and recovery of Li and Co from the spent LIBs using subcritical nickel-containing water is an inexpensive, efficient, sustainable and eco-friendly technology.

CAS / MDL: 872-50-4
研究领域: 环境科学 · 材料科学
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ChemCatChem · 2021 ·Vol. 13 ·期 8 ·2074-2085 · IF 5.686

Direct Amination of Biomass-based Furfuryl Alcohol and 5-(Aminomethyl)-2-furanmethanol with NH3 over Hydrotalcite-derived Nickel Catalysts via the Hydrogen-borrowing Strategy

Kuo Zhou,Ruihong Xie,Meiting Xiao,Darun Guo,Zhuodi Cai,Shimin Kang,Yongjun Xu,Jinjia Wei

Graphical Hydrogen borrowing : An efficient NiAl hydrotalcite-derived nickel catalyst has been developed for the direct amination of biomass-based furfuryl alcohol and 5-(aminomethyl)-2-furanmethanol with NH 3 via the “hydrogen borrowing” strategy. The synergistic catalysis of Ni 0 and Al δ+ -Al-O δ− site was of vital importance for the amination of alcohols into corresponding primary amines. A series of hydrotalcite-derived nickel catalysts were synthesized and employed for the direct amination of biomass-based furfuryl alcohol with NH 3 via the hydrogen borrowing strategy. The effects of the Ni/Al molar ratio and calcination temperature of the NiAl hydrotalcite-like precursors on the performance of the Ni x Al-CT catalyst were investigated. The systematic characterization showed that the synergistic catalysis of the metal and acid-base sites was of vital importance for the amination of alcohols. In particular, the Ni 2 Al-600 catalyst with high amount of Ni 0 sites (1.26 mmol g −1 ) and suitable density of acid-base sites (0.71 mmol g −1 and 1.10 mmol g −1 , respectively) exhibited the best dehydrogenation capability and therefore excellent catalytic activity. An 84.1 % yield of furfurylamine with complete conversion of furfuryl alcohol was obtained under the reaction conditions of 180 °C and 0.4 MPa NH 3 in 36 h. The presence of Ni 3 N in the spent catalyst, confirmed by XRD, TEM and XPS characterizations, was demonstrated to be responsible for the deactivation of the Ni x Al-CT catalyst. In addition, the Ni 2 Al-600 catalyst exhibited satisfactory performance toward another important biomass-related transformation of 5-(aminomethyl)-2-furanmethanol to 2,5-bis(aminomethyl)furan, with a yield of 70.5 %.

研究领域: 化学工程 · 催化科学
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CATALYSIS COMMUNICATIONS · 2019 · IF 3.674

Heterogeneous chitosan@nickel (II)-catalyzed tandem radical cyclization of N-arylacrylamides: A general method for constructing fluorinated 3,3-disubstituted oxindoles using perfluoroalkyl iodides

Haifeng Wu,Min Zhou,Wanmei Li,Pengfei Zhang

The first example of heterogeneous chitosan supported nickel (II) catalyzed tandem radical cyclization of N -arylacrylamides with perfluoroalkyl iodides is described. This approach provides a simple and efficient way to construct a variety of perfluoroalkylated oxindoles in good to excellent yields, with the advantages of readily available starting materials and easily recoverable heterogeneous catalyst. In addition, the highly active chitosan@nickel (II) catalyst was still active after being recycled six times.

CAS / MDL: 9012-76-4
研究领域: 有机化学 · 催化化学
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Materials · 2022 ·Vol. 15 ·期 9 ·3044 · IF 3.748

Improving Anti-Coking Properties of Ni/Al2O3 Catalysts via Synergistic Effect of Metallic Nickel and Nickel Phosphides in Dry Methane Reforming

Yu Shi,Shiwei Wang,Yiming Li,Fan Yang,Hongbo Yu,Yuting Chu,Tong Li,Hongfeng Yin

A series of NiP-x/Al2O3catalysts containing different ratio of metallic nickel to nickel phosphides, prepared by varying Ni/P molar ratio of 4, 3, 2 through a co-impregnation method, were employed to investigate the synergistic effect of metallic nickel-nickel phosphides in dry methane reforming reaction. The Ni/Al2O3catalyst indicates good activity along with severe carbon deposition. The presence of phosphorus increases nickel dispersion as well as the interaction between nickel and alumina support, which results in smaller nickel particles. The co-existence of metallic nickel and nickel phosphides species is confirmed at all the P contained catalysts. Due to the relative stronger CO2dissociation ability, the NiP-x/Al2O3catalysts indicate obvious higher resistance of carbon deposition. Furthermore, because of good balance between CH4dissociation and CO2dissociation, NiP-2/Al2O3catalyst exhibits best resistance of carbon deposition, few carbon depositions were formed after 50 h of dry methane reforming.Keywords:dry methane reforming;nickel catalysts;phosphides;coke-resistance;synergistic effect

CAS / MDL: 7783-28-0
研究领域: 催化 · 化学工程 · 材料科学
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FUEL · 2022 · IF 8.035

Effect of Ni/Al2O3 mixing on the coking behavior of bio-oil during its pyrolysis: Further understanding based on the interaction between its components

Zengtong Deng,Syed Shatir A. Syed-Hassan,Yuanjing Chen,Long Jiang,Jun Xu,Song Hu,Sheng Su,Yi Wang,Jun Xiang

Bio-oil can be converted to chemicals, carbon material, or syngas by various thermochemical processes which are always preceded with the pyrolysis step. In bio-oil pyrolysis, coke formation is almost inevitable, causing difficulties for further processing. In this study, bio-oil was mixed with Ni/Al 2 O 3 before it was fed for pyrolysis. Interesting results were observed whereby the effect of Ni/Al 2 O 3 mixing on coke formation shifted from promoting to inhibiting with increasing pyrolysis temperature. When the temperature was higher than 700 °C, contrary to the cases without mixing, the apparent decreases in coke yield were observed (e.g., the coke yield decreased by 10% at 800 °C). Comparative studies on bio-oil and its lignin-derived oligomer fraction indicated that the catalytic cracking of small molecules could enhance the formation of hydrogen radicals, which promoted thermal decomposition of lignin-derived oligomers, thus inhibiting coke formation via polymerization.

CAS / MDL: 1344-28-1
研究领域: 能源科学 · 催化化学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2022 ·Vol. 24 ·期 45 ·27923-27929 · IF 3.945

Compressive strain induced superior HER performance of nickel in alkaline solution

Zechen Xiao,Zhi Li,Yuhan Jing,Ting Li,Dongyang Jiang,Yuxian Duan,Qianxu Ye,Liexing Zhou,Anran Chen,Jinming Cai

The HER requires a highly efficient, cost-effective, and stable catalyst to adapt to the large-scale hydrogen industry. Nickel has been confirmed to be useful to drive the water splitting reaction, but the intrinsic performance remains unsatisfactory. In this work, nickel (EG–Ni) with compressive strain was prepared through a one-step electrochemical deposition strategy. It shows an outstanding enhancement for the HER, and it achieves a current density of 10 mA cm−2 at a low overpotential of 85.9 mV. A long-term durability test proves that the EG–Ni can tolerate a large current density of 100 mA cm−2, and the overpotential remains steady without dramatically increasing. Such a low overpotential and superior stability are attributed to the optimized adsorption energy on the catalyst surface, as evidenced by the downshifted position of the d-band center.

研究领域: 材料科学 · 电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Boron pretreatment promotes phosphorization of FeNi catalysts for oxygen evolution

Chendong Kou,Jieshu Zhou,Haibin Wang,Jingrui Han,Mei Han,Alberto Vomiero,Yongchang Liu,Hongyan Liang

Oxygen evolution reaction (OER) is a crucial half-reaction for many energy conversion technologies, which requires efficient catalysts to boost its sluggish kinetics. Herein, the FeNi catalyst with a high phosphating level (HP-Fe x Ni 2−x P) is constructed by a three-step synthetic route: (i) hydrothermal deposition of lamellar sheets, (ii) NaBH 4 pretreatment, and (iii) in situ phosphorization. FeNi layered double lamellar hydroxides were synthesized as the pre-catalysts. Then NaBH 4 pretreatment was used to remove the oxide impurities and introduce oxygen vacancies to promote phosphorization in the subsequent process. Finally, HP-Fe x Ni 2−x P nanosheets were achieved, with several advantages like abundant exposed active sites, high conductivity, and accessible mass transport channels. During the OER process, FeNiOOH/HP-Fe x Ni 2−x P interfaces are formed through spontaneous electrochemical activation and surface reconstruction. Benefitting from the synergistic interfacial effect and abundant exposed active sites, the NiFe based catalysts show an overpotential of ≈ 208 mV to reach 10 mA cm −2 in 1 M KOH, and a stability of 200 h at 1 A cm −2 . Overall, this work reports the rational design and preparation of a highly active OER catalyst, but also provides a general route through NaBH 4 pretreatment, which can be usefully applied to promote phosphorization in other systems of interest for catalytic applications.

研究领域: 材料科学 · 电化学
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