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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 47 ·期 15 ·7399-7409 · IF 3.3

Facile and scalable synthesis of 2D porous Ni/C via a salt-template assisted approach for enhanced urea oxidation reaction and energy-saving hydrogen production

Fengjiao Li,Xiaoming Zhang,Shuting Liang,Mingjuan Sun,Xiaolin Zhao,Haiwei Chen,Yanhui Cui

Urea splitting has gained increasing attention for energy-saving hydrogen production. The development of inexpensive, efficient and durable nanostructured electrocatalysts is highly desired to overcome the sluggish kinetics of the urea oxidation reaction (UOR). Nickel-containing materials have emerged as inexpensive and promising electrocatalysts for UOR in recent years. Herein, a series of cost-effective composites consisting of different loadings of Ni nanoparticles anchored on two-dimensional (2D) porous carbon nanosheets (denoted as Ni/CS) were fabricated for UOR via a facile and eco-friendly salt template-assisted approach. Among the prepared Ni/CS composites, the 4-Ni/CS sample with a suitable nickel loading and optimum structures exhibited the best UOR performances with a low potential of 1.369 V vs. reversible hydrogen electrode (RHE) at the current density of 10 mA cm−2 and a low Tafel slope of 39 mV dec−1. Furthermore, an overall urea splitting cell with the optimized 4-Ni/CS as the anode catalyst delivered only 1.372 V at 10 mA cm−2, which was 200 mV lower than the pure water splitting cell. The enhanced performances of 4-Ni/CS for UOR and the urea splitting cell were mainly attributed to its larger electrocatalytic specific area, more abundant active sites and defects, and faster mass transfer. The remarkable 2D porous 4-Ni/CS electrocatalyst exhibits potential application in UOR and energy-saving hydrogen production.

研究领域: 材料科学 · 电化学 · 能源工程 · 催化
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NANOTECHNOLOGY · 2023 ·Vol. 34 ·期 14 ·145704 · IF 3.5

Graphene-like wrapped Ni@C catalyst with magnetic recyclability for selective hydrogenation of nitro-aromatics

Jin Tan,Ling Lan,Yan-ni Wu,Song-bai Qiu

The graphene-like wrapped Ni@C catalysts were facilely synthesized by a modified sol–gel method. Nickel nitrate and citric acid (CA) were adopted as the raw materials to form sol–gel mixture. Under the circumstances, the additive CA were employed not only as a complexing agent but also as a carbon source. It is found that the calcination temperature and the mole ratios between Ni and CA are the key factors affecting the physical property and the catalytic performance of catalysts in the conversion of nitroarenes into corresponding anilines. The results show that the Ni@C-500(1:1) catalyst exhibited the best performance in the hydrogenation of o-chloronitrobenzenes (o-CNB) to o-chloroanilines (o-CAN). The yield of o-CAN was achieved at 100% when o-CNB was completely converted at 40.0 °C under 2.0 MPa H2 for 2.0 h. Furthermore, the Ni@C-500(1:1) catalyst could be separated and recovered easily after reaction by an external magnetic field. The investigated results indicate that the Ni@C-500(1:1) catalyst remained higher activity after using twelve times. More importantly, this kind of catalyst is also active for the selective hydrogenation of other nitroarenes into the corresponding anilines. This new synthetic method may pave a way for producing low-cost Ni@C catalysts on a large scale, which is attractive for industrial anilines applications.

研究领域: 化学工程 · 材料科学 · 催化 · 有机化学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

MOF-templated fabrication of Ni@C/g-C3N4 catalyst with high-dense accessible active sites achieving dicyclopentadiene hydrogenation at ambient conditions and comprehensive mechanism insight

Chenghong Wu,Xiaopeng Chen,Jiezhen Liang,Jiawei Fu,Zhongyao Zhang,Xiaojie Wei,Linlin Wang

The catalytic hydrogenation of dicyclopentadiene (DCPD) is one of the pivotal processes in the production of green high-energy-density liquid hydrocarbon fuels, jet propellent-10 (JP-10). However, the high dependency of the current catalysts on high temperature and pressure, whether the non-noble (>120 ℃, >15 bar) or even the noble catalyst (80 ℃, >7.6 bar), leads to enormous energy consumption and technical challenges in environment and sustainable development. Herein, we prepared a carbon layer wrapped Ni nanoparticles/g-C 3 N 4 catalyst (Ni@C/g-C 3 N 4 ) derived from the in-situ-formed Ni-MOF/g-C 3 N 4 composite. Benefiting from the 53.2 wt% small-sized Ni nanoparticles and nanosheet structure, resulting in high-density accessible active sites (5.38 × 10 20 sites g −1 ) and the mass transfer enhancement, Ni@C/g-C 3 N 4 achieved DCPD hydrogenation under ambient conditions. > 99.9 % DCPD conversion and 98.1 % endo -tetrahydrodicyclopentadiene yield was obtained at 30 ℃, 1 bar, significantly outperforming the benchmark 5 % Pd/C. To the best of our knowledge, it’s the mildest condition for DCPD hydrogenation. Further, comprehensive mechanistic insights were gained from combining means of kinetic investigations, in situ characterization, and theoretical calculations. The discrimination result of 27 kinetic models indicated that DCPD hydrogenation followed the Langmuir-Hinshelwood-Haugen-Watson formulism regarding the reaction between the chemisorbed dihydrodicyclopentadiene (DHDCPD) and dissociatively adsorbed hydrogen as the rate-determining step. In-situ DRIFTS confirm that the norbornene ring is preferentially adsorbed and hydrogenated. The DFT calculations further substantiate the hydrogenation pathway. The present work provides guidance for the development of highly efficient non-noble metal catalysts and opens up an environmental-friendly and economically viable avenue for DCPD hydrogenation.

研究领域: 催化 · 材料科学 · 化学工程 · 物理化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Indium-vacancy-rich In2S3/Ni@C photocatalyst with chemical bonds for producing hydrogen and benzylamine oxidation

Yuxin Liu,Yiqiang He,Chunguang Li,Zhan Shi,Shouhua Feng

Photocatalytic technology is considered a sound solution to exploit hydrogen energy. Currently, photocatalytic hydrogen production and organic synthesis under simulated sunlight simultaneously have enormous practical significance. Herein, we synthesized Ni@C metal nanoparticles cocatalyst to form a composite photocatalyst with Indium-vacancy-rich In 2 S 3 by the electrostatic self-assembly method. The composite exhibited a hydrogen production rate of 3.52 mmol·g −1 ·h −1 and coupling of benzylamine 8.37 mmol·g −1 ·h −1 . X-ray photoelectron spectroscopy and density functional theory explored the reaction process and mechanism. The charge density difference of the heterojunction surface revealed that the Ni@C interacted with the substrate via both electrostatic interaction and chemical bonds. This confirmed that the electrons rapidly transferred to the cocatalyst under the irradiation of visible light, which was conducive to the surface reduction reaction and greatly inhibited the photogenerated carrier recombination. Moreover, hydrogen adsorption energy further explained the synergistic effect of co-modification of the defect and the fact that noble-metal-free cocatalyst could improve photocatalytic efficiency. This work offers insights into the preparation of new types of photocatalysts which produce hydrogen and high-value chemicals in the future.

CAS / MDL: 22519-64-8
研究领域: 材料科学 · 化学工程 · 催化 · 能源材料 · 光化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Carbon-embedded Ni catalysts for highly efficient CO2 methanation

Zhihao Liu,Yachao Li,Kangzhou Wang,Yan Li,Yurong He,Jie Liang,Jianli Zhang,Tian-sheng Zhao,Noritatsu Tsubaki,Xinhua Gao

The design and preparation of highly active and stable Ni-based catalysts has attracted extensive attention. In this study, a series of embedded Ni@C catalysts were synthesized by a facile sol-gel method. After reduction at 400 °C, the optimized Ni@C-400 catalyst showed excellent performance in CO 2 methanation at a low temperature of 300 °C, with a CO 2 conversion of 74.3 % and good stability for 70 h. The characterization results indicated that after reduction treatment, the carbon species in the precursor were transformed into graphite carbon with more disorder defects. This structure facilitated the anchoring effect of the nickel components in the Ni@C catalyst, thereby forming a distinctive embedded structure that ensured the preservation of the nickel active phase in the catalyst following prolonged reaction. Therefore, the Ni@C catalyst prevented severe sintering and loss of loaded nickel. In addition, the interaction between Ni and C facilitated charge transfer, enhancing the CO 2 activation.

研究领域: 催化材料 · 化学工程 · 纳米技术
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EUROPEAN POLYMER JOURNAL · 2023 · IF 6

Self-healing polyurethane composite films loaded with Ni@C nanoparticles

Kaizhen Wan,Yue Cai,Qihui Chen,Maochun Hong,Zhao-Xi Zhou,Heqing Fu

Widely employed as polymers, polyurethanes also struggle to strike a balance between mechanical and self-healing qualities. Extrinsic self-healing can readily result in the production of material defects and stress concentration, which can result in the loss of mechanical property. In this study, self-healing and mechanical properties were combined to create a self-healing polyurethane nanocomposite film (PUHN) with good fatigue resistance. Reversible hydrogen and disulfide bonds were introduced to the polyurethane film, meanwhile, carbon-coated nickel nanoparticles were dispersed into the matrix as fillers during the early stage of polymerization. The results showed that PUHN combines outstanding mechanical properties with excellent self-healing properties, while the tensile strength of PUHN was increased by 38 % to 2.32 MPa due to the small-size effect caused by the introduction of nanoparticles. The introduction of reversible disulfide bonding and the presence of abundant hydrogen bonding give PUHN excellent self-healing properties, which can reach 91.2 % self-healing efficiency after 3 h in an oven at 80℃. Meanwhile, the fatigue resistance of the composite material also shows considerable application potential for use in packaging.

研究领域: 材料科学 · 纳米技术 · 高分子科学
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Catalysts · 2016 ·Vol. 6 ·期 5 ·63 · IF 2.964

Nickel Catalyzed Conversion of Cyclohexanol into Cyclohexylamine in Water and Low Boiling Point Solvents

Yunfei Qi,Haiyun Yu,Quan Cao,Bo Dong,Xindong Mu,Aiqing Mao

Nickel is found to demonstrate high performance in the amination of cyclohexanol into cyclohexylamine in water and two solvents with low boiling points: tetrahydrofuran and cyclohexane. Three catalysts, Raney Ni, Ni/Al2O3and Ni/C, were investigated and it is found that the base, hydrogen, the solvents and the support will affect the activity of the catalyst. In water, all the three catalysts achieved over 85% conversion and 90% cyclohexylamine selectivity in the presence of base and hydrogen at a high temperature. In tetrahydrofuran and cyclohexane, Ni/Al2O3exhibits better activity than Ni/C under optimal conditions. Ni/C was stable during recycling in aqueous ammonia, while Ni/Al2O3was not due to the formation of AlO(OH).Keywords:nickel;cyclohexanol;cyclohexylamine;base;hydrogen

CAS / MDL: 629-11-8
研究领域: 化学工程 · 催化 · 有机化学
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CARBON · 2022 · IF 11.307

Hierarchical carbon nanotubes@Ni/C foams for high-performance microwave absorption

Dawei Liu,Lei Yang,Fengyuan Wang,Hao Zhang,Jia Liu,Tong Lv,Hongjie Zhao,Yunchen Du

The construction of special three-dimensional microstructure is becoming an extremely fascinating approach to upgrade the electromagnetic properties of carbon-based microwave absorption materials (MAMs) recently. Herein, we have demonstrated the successful fabrication of a series of carbon nanotubes (CNTs)@Ni/C foams (CNCFs) through two-step pyrolysis processes . It is found that the loading amount of CNTs has an obvious influence on modulating the electromagnetic diameters of CNCFs, and thus effectively tuning their microwave absorption properties . With the relative carbon content of 66.3 wt%, CNCFs-2 exhibits admirable microwave absorption performance , including the effective absorption bandwidth of 5.8 GHz with the absorber thickness of 1.8 mm and the maximum reflection loss intensity of −47.0 dB therein. Electromagnetic analysis reveals that the intrinsic attenuation ability, well-matched characteristic impedance , and multiple reflection effect synergistically work for the excellent reflection loss characteristics of CNCFs-2, which indicates rational microstructure design and appropriate chemical composition regulation are vitally important for the enhancement of microwave absorption performance. We believe these desirable microwave absorption properties can make CNCFs-2 eligible to be a very promising candidate for high-performance MAMs, and this research will provide some inspirations more or less for the development of more advanced carbon-based MAMs in the future.

CAS / MDL: 25249-54-1 9003-39-8
研究领域: 材料科学 · 电磁学 · 化学工程
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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

N-Doped 3D Porous Ni/C Bifunctional Electrocatalysts for Alkaline Water Electrolysis

Jieting Ding,Shan Ji,Hui Wang,Vladimir Linkov,Hengjun Gai,Fusheng Liu,Quanbing Liu,Rongfang Wang

Water electrolysis offers a promising approach toward future sustainable energy mix utilizing hydrogen as energy carrier. Bifunctional catalyst which is active in both oxygen and hydrogen evolution reactions can significantly enhance total electrochemical water splitting efficiency and simplify electrolysis systems. In this study, nitrogen doped nickel-containing porous carbon networks were prepared to fulfill this role. Peptone was used as carbon and nitrogen source during the synthesis and NaCl presence as a template resulted in the formation of open mesopores interconnected by thin carbon sheets with nanosized Ni particles encapsulated in the carbon matrix. A low onset potential of 53 mV and a charge transfer resistance of 3.8 Ω with excellent cycling stability were demonstrated when the optimized catalyst Ni-2 was applied in HER. It was also shown that Ni-2 onset potential, charge transfer resistance, and durability in OER were comparable to those of a commercial RuO2 catalyst. During the electrolysis study conducted at 10 mA cm–2, Ni-2 maintained a cell voltage of 1.63 V with remarkable stability during 25 h operation.

研究领域: 电化学 · 材料科学 · 能量转换 · 催化 · 氢能
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

Tunable interlayer spacings Ti3C2Tx MXene/Ni/C for enhanced electromagnetic microwave absorption

Jingyu Song,Yongqian Shen,Guibin Zhang,Mingxuan Sun,Mengyao Han,Xueyan Du

While two-dimensional lamellar materials, specifically Ti 3 C 2 T x MXenes, have shown great promise as wave-absorbing materials, the precise design of interlayer spacing poses a persistent challenge. In this study, Ti 3 C 2 T x MXene layers with adjustable interlayer spacings were crafted using a straightforward molecular welding technique. Through the incorporation of Ni nanoparticles onto the Ti 3 C 2 T x MXene layers using a combination of simple mechanical stirring and carbonation reactions, we successfully developed Ti 3 C 2 T x MXene/Ni/C composites featuring a distinct lamellar structure. A uniform dispersion of Ni nanoparticles on the surface of the Ti 3 C 2 T x MXene nanosheets was found with some of the nanoparticles intercalated into the layers. The Ti 3 C 2 T x MXene/Ni/C composites exhibited a maximum reflection loss (RL) value of −42.3 dB at 12.3 GHz, accompanied by an impressive effective absorption bandwidth (EAB) of 5.6 GHz. This outstanding absorption performance could be attributed to various factors, including the dielectric loss of the Ti 3 C 2 T x MXene lamellae, reflections and scattering of multiphase heterostructures, the magnetic loss of the Ni nanoparticles, and their synergistic attenuation. Furthermore, Ni nanoparticles with high electrical conductivity induced vortex currents under the alternating influence of electromagnetic waves (EMWs), resulting in a substantial depletion. This study introduces an innovative approach for synthesizing Ti 3 C 2 T x MXene/Ni/C composites with tunable interlayer spacing, showing their potential for applications in microwave absorption (MA).

研究领域: 材料科学 · 电磁学
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ENERGY & FUELS · 2024 · IF 5.2

Hydrogenation of Dicyclopentadiene over Stable SiO2@Ni/C Catalysts under Mild Conditions

Dandan Jia,Jie Zhao,Rui Yan,Hongyi Gao,Zhaolin Fu,Zhongpeng Zhu,Zhiping Tao

The catalytic stability has always been a bottleneck of many reactions in industrial production. The preparation of long-life hydrogenation catalysts has been a hot research topic. Herein, Ni-ZIF was first grown in situ on the surface of SiO2. N-doped Ni/C nanoparticles were uniformly distributed on the SiO2 support after the subsequent annealing process. The uniform dispersion of Ni-ZIF contributed to the high dispersion of the active metal, and the highly dispersed Ni nanoparticles were free from thick carbon layers. The highly dispersed and fully exposed Ni determined its excellent low-temperature hydrogenation activity, which was critical for the extension of the catalyst lifetime. The presence of carbon and nitrogen was also beneficial to improve the stability of the catalyst. The N-doped SiO2@Ni/C catalyst exhibited excellent stability toward the hydrogenation of DCPD under mild condition. 100% DCPD conversion and >90% THDCPD selectivity were maintained after 144 h of continuous fixed-bed operation under GHSV of 2 h–1 at 60–90 °C.

研究领域: 催化化学 · 材料科学
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Reaction Chemistry & Engineering · 2019 ·Vol. 5 ·期 1 ·58-65 · IF 3.935

Biomass-derived carbon-supported Ni catalyst: an effective heterogeneous non-noble metal catalyst for the hydrogenation of nitro compounds

Qingjie Tang,Ziliang Yuan,Shiwei Jin,Kaiyue Yao,Hanmin Yang,Quan Chi,Bing Liu

There has been a great deal of attention to the development of heterogeneous non-noble metal catalysts for the selective and mild hydrogenation of nitro compounds into primary amines. Herein, a biomass-derived carbon material supported Ni catalyst (Ni/C) was facilely prepared by a one-pot pyrolysis process, and the as-prepared Ni/C catalyst demonstrated a high catalytic activity for the hydrogenation of nitro compounds into primary amines at room temperature. The Ni/C catalyst not only demonstrated a high catalytic activity but also showed a good tolerance to other functional groups. Structurally diverse primary amines were achieved in yields from 92% to 99% within a few hours at room temperature under 5 bar H2. Furthermore, the Ni/C catalyst showed good reusability without the loss of its activity.

研究领域: 催化化学 · 材料科学 · 有机合成
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