SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Wen-Jian Yang,Li-Hui Yang,Han-Jun Peng,Si-Hao Lv,Hafiz Muhammad Adeel Sharif,Wei Sun,Wei Li,Cao Yang,Hui Lin
Electroreduction removal of nitrate (NO 3 – -N) is considered as a promising approach to solve its adverse effects on environment and human health, where efficient and cheap catalysts are required. Perovskite-based catalysts showed a versatile catalytic ability for wide range of redox reactions, but seldom applied for NO 3 – -N reduction. Herein, four perovskite oxide cathodes, LaMO 3-δ (M = Fe, Co, Ni and Cu) were prepared and used for the reduction of NO 3 – -N. The Ruddlesden-Popper (RP) type La 2 CuO 4 exhibited the best NO 3 – -N catalytic activity among the four perovskite oxide cathodes, with a removal rate of 11.7 × 10 -3 min −1 . The high selectivity of NH 4 + -N (82.4 ± 2.2%) indicated that NH 4 + -N was the main final product for NO 3 – -N electroreduction at La 2 CuO 4 cathode, but 100% of N 2 selectivity could be obtained with addition of 1000 and 1500 mg/L Cl - as the electro-assisted chlorination process. The mechanism of NO 3 – -N electroreduction occurred by both electron- and H*-mediated pathway, and the oxygen vacancies and redox cycle of Cu(I)-Cu(II)-Cu(I) were proposed as the accommodation sties and direct electron sources for NO 3 – -N reduction. Generally, this study opens a novel avenue for the development of earth-abundant, cost-effective catalyst with effective NO 3 – -N electroreduction.
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高影响因子
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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Molecular Catalysis
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2022
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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 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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EcoMat
·
2022
·Vol. 4
·期 2
·e12164
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IF 12.213
Chaoyu Lin,Gan Luo,Huiqin Zhou,Anlin Feng,Li Zeng,Qingyang Li
An amorphous Ni nanoparticles-loaded ZnO nanowire array is controllably constructed on stainless steel mesh through combined electrodeposition and hydrothermal reaction. Its nano-arrayed structure not only provides a platform to achieve stable and good dispersion of Ni nanoparticles, but also helps improve their ability to adsorb 4-nitrophenolate ions and to capture hydrogen radicals, thereby accelerating the hydrogen transfer from metal hydride complex to 4-nitrophenol. Benefiting from the abovementioned unique features, it outperforms most Ni-based catalysts. While a 30-s re-electrodeposition of Ni can provide it extra 150 min of high catalytic activity towards the reduction of waste 4-nitrophenol to valuable 4-aminophenol, further demonstrating its outstanding reusability. The highly general methodology reported here paves the way to economically and effectively synthesize various other metal nanoparticles-loaded ZnO nanowire arrays on different conductive substrates, which not only enrich the nanowire-arrayed catalysts, but also significantly promote their practical utilizations in a wide range of environment-related fields.
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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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Journal of Materials Chemistry A
·
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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Reaction Chemistry & Engineering
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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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Nanomaterials
·
2022
·Vol. 12
·期 5
·729
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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
ACS Catalysis
·
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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ENERGY & FUELS
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2022
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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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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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