Journal of Energy Storage
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2022
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IF 8.907
Jiahui Fan,Aiying Chen,Xiaofeng Xie,Lijian Gu
Three-dimensional (3D) hybrids are very valuable in the construction of supercapacitor electrodes. Ni(OH) 2 cellular arrays were in-situ grown on nickel foam using Co 3 O 4 nanosheets (NSs) as nucleating agent. The formation, microstructure and supercapacitance performance of the Co 3 O 4 /Ni(OH) 2 cellular arrays are systematically investigated. The Co 3 O 4 /Ni(OH) 2 arrays present an open cellular nanostructure with ultrathin Ni(OH) 2 walls. The Co 3 O 4 /Ni(OH) 2 prepared by hydrothermal reaction of 12 h delivers a super-high specific capacitance of 4396 F g −1 at 1 A g −1 , above the theoretical capacitances of both the Ni(OH) 2 and Co 3 O 4 . Additionally, the Co 3 O 4 /Ni(OH) 2 electrode shows an excellent cycle performance by retaining 80.1% after 5000 cycles and a stable rate capability by decreasing 21.1% from 1 to 10 A g −1 . The assembled asymmetric supercapacitor reaches a large energy density of 32 Wh kg −1 at 7999 W kg −1 by Co 3 O 4 /Ni(OH) 2 as anode and reduced graphene oxides as cathode. The prominent high-capacity performance can be attributed to the cellular arrays, ultrathin hybrid NSs and synergetic reactions of the Ni(OH) 2 and Co 3 O 4 . The proposed technology is also suitable for producing other multi-component oxide/hydroxide arrays as electroactive materials for energy storage devices.
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ACS Catalysis
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2022
·
IF 13.7
Shuangxi Lin,Qiang Wang,Maoshuai Li,Ziwen Hao,Yutong Pan,Xiaoyu Han,Xiao Chang,Shouying Huang,Zhenhua Li,Xinbin Ma
Controlling the selectivity of CO2 hydrogenation by catalysis is a fundamental challenge. This study examines the interrelation between active sites and reaction pathways in Ni-catalyzed CO2 hydrogenation. The alloying of Ni with Zn to charged (Niσ––Znσ+) active sites modifies the electronic structure and d-band center, weakens the interaction with CO/H2, and preferentially catalyzes the reverse water gas shift to CO with the thermodynamically favored methanation pathway switched off. The charged dual sites can stabilize the activated CO2 species in a η2(C, O) bridge configuration, directly dissociate the C═O bond to *CO, and promote CO desorption. The mechanistic investigation has elucidated the reaction pathways in the Ni-catalyzed CO2 hydrogenation and identified the crucial intermediates that impacted the product selectivity, which can provide a theoretical guide for the Ni-based catalyst design.
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Reaction Chemistry & Engineering
·
2022
·Vol. 7
·期 5
·1126-1135
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IF 5.2
Shanshan Lin,Jianguo Liu,Longlong Ma
The catalytic hydrogenation of organic substrates containing plenty of unsaturated functional groups is an important step in the industrial preparation of fine chemicals and has always been a hot spot in basic catalysis research. For example, phenylethanol obtained by the preferential hydrogenation of the CO group of acetophenone is a valuable intermediate for the production of spices, flavors, and medicines. Furthermore, as the demand for 1-phenylethanol (PhE) continues to increase, the catalytic hydrogenation of acetophenone (AP) is becoming more and more important. At present, relatively few catalytic systems are used in this reaction as the hydrogenation of acetophenone is a complex multi-step reaction. Enantioselective hydrogenation on heterogeneous catalysts is remarkable due to its inherent operational and economic advantages, such as atom economy. It is one of the most ideal methods as the catalyst is easily separated and recycled. However, the traditional synthesis way in batch reactors usually takes a long time with unsatisfactory conversion which is not conducive to industrialization. Heterogeneous non-precious metal catalysts are advantageous for their implementation in flow reactor systems for industrial applications due to their ease of separation, low cost, and environmental friendliness. Herein, we report the first use of non-noble metal Ni-supported graphene-based catalysts for hydrogenation of acetophenone to phenylethanol with high efficiency in a flow reactor made of 316L stainless steel with a length of 200 mm and an inner diameter of 6 mm which can significantly improve mass and heat transfer. The conversion rate under the optimized reaction conditions can reach 99.14% with a satisfactory selectivity of 97.77% (the conversion and selectivity are in mol%). The magnetic catalyst has a compact structure, and the Ni particles coated with carbon on the surface are uniformly distributed. After 48 hours of uninterrupted continuous experiments, the conversion rate of acetophenone still reached 88.44%. The catalyst has good cyclability, and the Ni-based catalyst after the cycle still maintains high catalytic activity without obvious deactivation, and the catalyst structure remains intact and stable.
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Journal of Materials Chemistry A
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2022
·Vol. 10
·期 12
·6560-6568
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IF 14.511
Yunqing Kang,Haoran Du,Bo Jiang,Hui Li,Yanna Guo,Mohammed A. Amin,Yoshiyuki Sugahara,Toru Asahi,Hexing Li,Yusuke Yamauchi
Supported amorphous alloy catalysts have received wide attention due to their unique structural and electronic properties, high catalytic activity, and thermal stability. In this work, a carbon nanotube (CNT)-supported amorphous Ni–P alloy nanoparticles (NPs) catalyst, referred to as Ni–P/CNTs-MA, is synthesized using a simple one-pot microwave-assisted approach. The prepared Ni–P/CNTs-MA catalyst displays smaller Ni–P NPs, higher metal dispersion and stronger metal–support interactions than the reference catalyst prepared by the traditional water bath heating method (Ni–P/CNTs-WB). The resulting Ni–P/CNTs-MA catalyst exhibits enhanced catalytic activity for the hydrogenation of nitroarenes compared to the Ni–P/CNTs-WB catalyst. The Ni–P/CNTs-MA catalyst also exhibits improved thermal stability and catalytic durability, probably due to the strong interaction between the Ni–P NPs and CNTs.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
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IF 3.898
Haocui Zhang,Zhourong Xiao,Mei Yang,Jijun Zou,Guozhu Liu,Xiangwen Zhang
Ni/SBA-15 modified by highly dispersed cerium-oxide was prepared with the aid of sucrose for steam reforming of JP10 (C 10 H 16 ). Their characterization showed that addition of appropriate amount ceria led to the formation of highly dispersed CeO 2 and Ni, and the CeO 2 covered smaller nickel particles like strawberry seeds to form much more interface between them. Their catalytic activity exhibited higher stability over time on stream of 6.5 h with conversion higher than 95% and higher carbon resistance (mass loss less than 4.5% by TG), which may derive from good properties below: (1) much more interface enhanced cooperation effect and increased turnover frequency at the interface; (2) the stronger interaction between Ni and ceria to suppress sintering by formation of Ni-O-Ce solid solution; (3) the large amount of oxygen vacancies from the formation of Ni-O-Ce solid solution and highly dispersed CeO 2 to facilitate the water–gas–shift reaction and carbon removal.
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Nanomaterials
·
2022
·Vol. 12
·期 5
·729
·
IF 5.719
Rui Zhang,Hengrui Qiu,Youxiang Zhang
The tungsten-doped (0.5 and 1.0 mol%) LiNi0.88Co0.09Al0.03O2(NCA) cathode materials are manufactured to systematically examine the stabilizing effect of W-doping. The 1.0 mol% W-doped LiNi0.88Co0.09Al0.03O2(W1.0-NCA) cathodes deliver 173.5 mAh g−1even after 100 cycles at 1 C, which is 95.2% of the initial capacity. While the capacity retention of NCA cathodes cycled in identical conditions is 86.3%. The optimal performances of the W1.0-NCA could be ascribed to the suppression of impendence increase and the decrease in anisotropic volume change, as well as preventing the collapse of structures during cycling. These findings demonstrate that the W-doping considerably enhances the electrochemical performance of NCA, which has potential applications in the development of Ni-rich layered cathode materials that can display high capacity with superior cycling stability.Keywords:tungsten doping;phase transition;structural stability;electrochemical performance;LiNi0.88Co0.09Al0.03O2
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PubMed
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-12
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IF 17.694
Ou Xing,Liu Tongchao,Zhong Wentao,Fan Xinming,Guo Xueyi,Huang Xiaojing,Cao Liang,Hu Junhua,Zhang Bao,Chu Yong S.,Hu Guorong,Lin Zhang,Dahbi Mouad,Alami Jones,Amine Khalil,Yang Chenghao,Lu Jun
High-capacity Ni-rich layered oxides are promising cathode materials for secondary lithium-based battery systems. However, their structural instability detrimentally affects the battery performance during cell cycling. Here, we report an Al/Zr co-doped single-crystalline LiNi 0.88 Co 0.09 Mn 0.03 O 2 (SNCM) cathode material to circumvent the instability issue. We found that soluble Al ions are adequately incorporated in the SNCM lattice while the less soluble Zr ions are prone to aggregate in the outer SNCM surface layer. The synergistic effect of Al/Zr co-doping in SNCM lattice improve the Li-ion mobility, relief the internal strain, and suppress the Li/Ni cation mixing upon cycling at high cut-off voltage. These features improve the cathode rate capability and structural stabilization during prolonged cell cycling. In particular, the Zr-rich surface enables the formation of stable cathode-electrolyte interphase, which prevent SNCM from unwanted reactions with the non-aqueous fluorinated liquid electrolyte solution and avoid Ni dissolution. To prove the practical application of the Al/Zr co-doped SNCM, we assembled a 10.8 Ah pouch cell (using a 100 μm thick Li metal anode) capable of delivering initial specific energy of 504.5 Wh kg −1 at 0.1 C and 25 °C.
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PubMed
高影响因子
ENERGY & FUELS
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2022
·
IF 4.654
Cheng Lan,Heping Xie,Yifan Wu,Bin Chen,Tao Liu
Electrochemical seawater splitting using efficient HER (hydrogen evolution reaction) and OER (oxygen evolution reaction) electrocatalysts have become an appropriate method for the mass production of green hydrogen. In this study, a noble-metal free OER electrocatalyst consisting of Mo-doped Ni3S2 nanocluster arrays on Nickle foam (Mo–Ni3S2/NF)─fabricated using a modified one-step solvothermal approach─is developed and evaluated. The proposed electrocatalyst demonstrates exceptional OER activity, requiring overpotentials of only 212 and 291 mV to deliver OER current densities of 10 and 100 mA cm–2, respectively, in alkaline seawater. The presence of Mo promotes Ni–S coordination, resulting in strong electronic interactions and substantially enhanced OER kinetics. Meanwhile, surface sulfate ions and (oxy)hydroxide (NiOOH) generated during the OER lead to enhanced activity and corrosion resistance, enabling Mo–Ni3S2/NF to operate continuously at 100 mA cm–2 for 500 h in alkaline natural seawater. This study is expected to inform the progression of sulfur-based transition-metal electrocatalysts for seawater oxidation.
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Molecular Catalysis
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2022
·
IF 5.089
Cong Wang,Gang Li,Hongchen Guo
Compared with the mainstream approaches of doping the active metal in the MOFs structure and post-synthetic modification, it is more convenient to directly use the coordinatively unsaturated metal sites of MOFs for catalytic reactions. Herein, two forms of Ni-MIL-77 (1D Ni-MIL-77 and 3D MIL-77) were prepared using one-pot method and characterized by ICP-AES, XRD, FT-IR, XPS and SEM. Among them, 1D Ni-MIL-77 without high temperature heat treatment exhibited a better heterogeneous catalytic ethylene dimerization activity that was up to 989.6 g pro. /(g cat. ·h) (TOF=5544 h −1 ) and the selectivity of 1-butene could reach 93.3% at the optimal conditions. In addition, a probable Cossee-Arlman-like mechanism was proposed. By studying the catalyst structure after reaction, it was found that the reason for limited reuse was the hydrolysis products of the co-catalyst covered the catalysts.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Xianping Ye,Jian Wu,Fenghua Chen
Fabrication of low-cost, stable and highly efficient catalysts for clean energy and environmental control applications is an urgent task. In this work, we have successfully synthesized a multifunctional two-dimensional rare earth-based LaOCl@hcp-Ni heterostructure via a simple one-pot method. Here, the semiconductor LaOCl nanoparticles were well deposited on the metastable metal hcp-Ni, and the hexagonal close-packed structure of hcp-Ni matched the layered-structure LaOCl to form a highly active LaOCl@hcp-Ni Schottky catalyst. Furthermore, LaOCl@hcp-Ni were tested for Photoelectrochemical (PEC) oxygen evolution reaction (OER) in alkaline media and the photocatalytic (PC) degradation of Rhodamine B (RhB) in aqueous solution. LaOCl@hcp-Ni shows excellent PEC-OER catalytic activity and RhB degradation performance under artificial simulated sunlight. This enhancement of PEC and PC performance is due to the Schottky interface constructed by the coupling of hcp-Ni and LaOCl, which generates an interface electric field to effectively promote the transfer of photogenerated electrons from the semiconductor LaOCl to the metal hcp-Ni through the interface. Thus, energy band gap of LaOCl with oxygen defects is adjusted to the visible light region and their valence state of La is lowered, realizing high-efficiency visible light catalytic activity. Thus, it would be a potential rare earth-based Schottky catalyst, which can be used for the PEC oxygen evolution and the PC degradation of organic pollutants.
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JOURNAL OF SOLID STATE CHEMISTRY
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2022
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IF 3.656
Xiaoya Kang,Jiawei Wang,Yingxia Ma,Xiaofeng Shi,Xinquan Chen,Hu Tian,Fen Ran
Metal-organic frameworks (MOFs) haves been intensively studied as active electrode materials for supercapacitors . However, few studies have been systematically investigated the electrochemical performance of MOFs as electrode materials by adjusting the raw material components and reaction conditions to regulate and control MOFs morphology structures. Herein, a series of nickel/cobalt MOFs (Ni/Co-MOFs) with different morphology structures were synthesized by one-pot solvothermal method via adjusting raw material components and reaction conditions. Results show that three-dimensional (3D) juniperus sabina-like Ni/Co-MOF has optimal electrochemical performance with a specific capacitance of 982.5 F/g at 0.5 A/g. Meanwhile, the asymmetric supercapacitor exhibits the capacitance of 132.0 F/g at 0.5 A/g, and the corresponding energy density and power density are 46.9 Wh/kg and 400.0 W/kg, respectively. The work presents a novel strategy to regulate and control the morphology structures of MOFs by adjusting the raw material components and reaction conditions to achieve the optimal electrochemical performance of MOFs.
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RENEWABLE ENERGY
·
2022
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IF 8.634
Yiwei Tang,Xiaoning Liu,Ran Xi,Le Liu,Xinhua Qi
As one of the important chemical feedstocks and biofuels, ethyl levulinate (EL) can be produced from biomass-derived furfural by consecutive hydrogenation, etherification and ring-opening reactions. However, this process normally requires two separate steps in different reaction systems, which is complex and energy consumption. Herein, Nb–Ni bifunctional ordered mesoporous carbons (Nb/ [email protected] ) were synthesized by a two-step process where [email protected] was firstly synthesized by a solvent evaporation induced self-assembly (EISA) process using F127 as a template agent, polyphenol gallic acid as carbon precursor and Ni 2+ as cross-linker, following with the supporting of Nb species in the [email protected] by an incipient wetness impregnation method. The as-synthesized Nb/ [email protected] samples were applied for the one-pot catalytic transformation of furfural to EL, and exhibited good activity with the highest EL yield of 83% under an optimized condition. Two possible pathways for the one-pot production of EL were proposed according to two intermediates: (1) hydrogenation of furfural to form furfuryl alcohol (FFA) that is then etherified with ethanol to form 2-(ethoxymethyl)furan (2-EMF); and (2) acetalization and etherification of furfural with ethanol to produce 2-(diethoxymethyl)furan (2-DMF). Then both 2-DMF and 2-EMF are converted to EL through acid catalyzed ring opening reaction. The dominant reaction pathway varied with the properties of the catalyst and the applied reaction conditions.
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