CATALYSIS TODAY
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2018
·
IF 4.667
Dawang Chu,Chen Zhao
The effective and selective conversion of cellulose to valuable fuels and chemicals is highly attractive. In this paper, we prepared a catalyst with the adjacent surface Cu° and oxygen-deficient WO x (2 < x < 3) species by reduction of CuWO 4 precursor, and such catalyst coupled with Ni/activated carbon (AC) attained high yield (71 wt%) and good cycling performances in catalyzing one-step hydrothermal conversion of cellulose to ethylene glycol (EG), highly superior to the performances on physically mixed Ni/C, Cu/C and WO 3 . The increased Cu doping amounts led to a higher ratio of the lower valence state W (V or IV) to the high valence W(VI) as indicated by XPS, XRD, and TPR-H 2 analyses. The oxygen vacancies on the hydrogen-reduced CuWO 4 sample dramatically increased, probably due to the benefits from the substantial dissociated H• on the neighboring Cu° center. The EG yields from cellulose are shown to be proportional to the concentrations of oxygen vacancies on WO x , which catalyzes the important elementary retro-aldol step reaction via adsorbing C 6 sugar intermediates in a specific way. It is inferred that Cu introduction is mainly used to create more oxygen vacancies on the WO x surface that helps adsorbing oxygenates, while Ni fast hydrogenates of hydroxyacetaldehyde to EG and avoids coking, constructing a multi-functional synergistic catalytic process from converting of cellulose to EG in the high-temperature water
研究领域:
催化化学
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生物质转化
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绿色化学
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材料化学
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能源化学
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JOURNAL OF ALLOYS AND COMPOUNDS
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2019
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IF 4.175
Jiawei Lin,Jun Deng,Zhongnan Guo,Erjian Cheng,Fan Sun,Ning Liu,Bianbian Wang,Shiyan Li,Wenxia Yuan
The materials with quasi-one-dimensional crystal structure have gained intense interest because of their novel structure and related properties such as electron correlations , charge-density wave and potential superconductivity . Here we report two new Ni-based quasi-one-dimensional selenides : Rb 0.9 Ni 3.1 Se 3 and K 0.7 Ni 3.1 Se 3 . These two compounds are nonstoichiometric and composed of one-dimensional (Ni 3 Se 3 ) ∞ infinite chains with face-sharing Ni 6 octahedra along the c direction. It is found that the interchain distance in these compounds is strongly influenced by the radius of intercalated alkali-metal cations, while the configuration of (Ni 3 Se 3 ) ∞ chains is basically unaffected. The conductivity measurement indicates the metallic behavior of Rb 0.9 Ni 3.1 Se 3 and K 0.7 Ni 3.1 Se 3 . Meanwhile, the magnetic susceptibility reveals the spin-glass state below 10 K. It is indicated that the magnetic moments in these compounds are related to the Ni Ni bonding distance. First-principles calculation reproduces the metallic state of this 133 phase, and also suggests that the magnetic interaction is attributed to the extra Ni in structure. These compounds form a Ni-based quasi-one-dimensional material family, which provides new platform to understand the structure-property relationship of quasi-one-dimensional materials, and also offer a series of potential precursors to synthesis the novel (Ni 3 Se 3 ) ∞ molecular wires .
研究领域:
凝聚态物理
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材料科学
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无机化学
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固体化学
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低维材料
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电子结构理论
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 18
·51876-51886
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IF 5.8
Yu Weiting,Zhu Jieyun,Chen Sizhuo,Tang Juntao,Ye Jiexu,Song Shuang
The electrocatalytic reduction of CO 2 towards CO is one of the most desirable routines to reduce atmospheric CO 2 concentration and maintain a global carbon balance. In this work, a novel porous NiCu-embedded ZIF-derived N-doped carbon nanoparticle (NiCu@NCNPs) catalyst has been identified as an active, highly selective, stable, and cost-effective catalyst in CO 2 reduction. A CO selectivity as high as 100% has been achieved on NiCu@NCNPs which is the highest reported to date. The particle current density of CO on NiCu@NCNPs is around 15 mA cm –2 under the optimized potential at −0.9 V vs. RHE. The NiCu@NCNPs electrode also exhibits excellent stability during the five sequential CO 2 electroreduction experiments. The superior catalytic performance of NiCu@NCNPs in CO 2 RR can be related to its microstructure with high electrochemical surface area and low electron transfer resistance. Furthermore, a kinetic analysis has shown the formation of intermediate *COOH is the rate-determining step in CO 2 RR towards CO. According to the results of density functional theory (DFT) calculations, a low Gibbs-free energy change (∆ G ) for the rate-determining step leads to the enhanced catalytic performance of CO 2 RR on NiCu@NCNPs.
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高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2023
·Vol. 27
·期 5
·1261-1268
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IF 2.5
Deng Hao-chen (Preston),Hao Qingzhu,Wang Yuhang
The COVID-19 pandemic that is still prevalent around the globe each day consumes massive disposable face masks and consequently lays a heavy burden on waste management. Meanwhile, the incineration of these medical wastes further escalates the already overwhelming carbon emission that leads to global warming and climate change. To offer a potential solution addressing medical waste and CO 2 emission challenges, we herein develop a synthetic protocol to upgrade face masks into Ni, N-doped graphene (Ni–N-C) sheet catalysts for selectively reducing CO 2 into CO electrochemically. The high specific surface area and the uniform dispersion of Ni active sites of the catalyst derived from a regular disposable face mask enable a near-unity CO Faradaic efficiency (FE) at the current density of 200 mA cm −2 . This study offers outside-of-the-box thinking to address environmental issues by turning medical wastes into CO 2 reduction catalysts.
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Molecular Catalysis
·
2023
·
IF 4.6
Sihao Shu,Zhongze Wang,Xing Zhang,Haonan Shi,Shangzhen Feng,Jixiang Chen
Al 2 O 3 supported Ni-Sn alloy (Ni/Sn atomic ratio of 6) and Ni 3 Sn, Ni 3 Sn 2 and Ni 3 Sn 4 intermetallic compounds (IMCs) were prepared by co-precipitation method for the deoxygenation of fatty acid methyl esters to produce hydrocarbons. In comparison with metallic Ni, the catalytic evaluation and methyl propionate-TPD/TPSR results reveal that Ni-Sn IMCs remarkably inhibit the decarbonylation/decarboxylation pathway, C-C bond hydrogenolysis and methanation while promote the hydrodeoxygenation pathway, subsequently enhancing the yield of aiming hydrocarbons. Therein, 20%Ni 3 Sn 2 /Al 2 O 3 has the best performance, and the hydrocarbons yield reach about 99% in the deoxygenation of methyl octanoate and methyl palmitate. We suggest that the geometric and electronic effects of Sn contribute the excellent performance of Ni-Sn IMCs, and there is synergetic effect between Ni and Sn sites for the activation of C-O/C=O bond, for which a suitable Ni-Sn atomic spacing is very important. Finally, the catalyst stability and deactivation were also investigated.
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Energy Technology
·
2023
·Vol. 11
·期 8
·2300118
·
IF 3.8
Peiyao Pan,Qingle Zeng,Xiaoxiao Li,Chao Liu,Jinming Zeng,Tongxiang Liang,Xiaopeng Qi
Electrocatalytic water splitting provides an effective way to store electrical energy (i.e., solar and wind energy) intermittently. It is believed that developing electrocatalysts with excellent stability, high catalytic efficiency, and abundant natural reserves is the key to the industrialization of electrochemical water splitting. Herein, nickel–molybdenum electrocatalyst formed on the surface of a low-cost etched stainless-steel mesh via a one-step electrodeposition method exhibits a low hydrogen evolution overpotential of 53 mV and oxygen evolution overpotential of 261 mV at a current density of 10 mA cm −2 due to the synergistic effect of nickel and molybdenum. Moreover, the as-prepared catalyst demonstrates superior hydrogen evolution reaction (HER) catalytic performance than commercial Pt/C at current density exceed 200 mA cm −2 . The electrocatalyst also shows excellent HER and oxygen evolution reaction stabilities at high current density attribute to the tightly bond between electrocatalyst and the etched stainless-steel mesh, as well as the surface reconstruction of catalyst during the cycle test. The facile electrodeposition method has lower requirements on production equipment, using stainless steel mesh as the basement reduces the production cost, the nickel–molybdenum alloy possesses excellent electrolytic water splitting performance and stability. These results indicate that this work can provide an idea for the industrialization of electrochemical water splitting.
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RARE METALS
·
2023
·Vol. 42
·期 7
·2284-2293
·
IF 8.8
Du Juan,Lin Qin-Yan,Zhang Jian-Qi,Hou Sen-Lin,Chen Ai-Bing
Herein, we successfully prepare highly dispersed and uniform small nano-size nickel nanoparticles embedded on core–shell carbon spheres by confined-deposition method. The mesoporous silica layer containing surfactant coated on the surface of the polymer sphere provides confined space and effectively controls the growth of nickel nanoparticles during pyrolysis. At the same time, the introduction of nickel species has an impact on structure of the obtained carbon spheres, and it can promote the deposition of carbon to realize the adjustment from hollow to core–shell and then to solid spheres. Owing to the uniform distribution of Ni nanoparticles with small size, mesoporous structure, N-doping groups, high specified surface areas, and core–shell structure, the obtained catalyst shows exciting ability for the production of CO by reduction of CO 2 with a maximum CO Faradaic efficiency of 98%, indicating its promising prospect in electro-reduction of CO 2 . Graphical Abstract
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Materials
·
2023
·Vol. 16
·期 8
·3079
·
IF 3.4
Lifan Wang,Qinling Shi,Chun Zhan,Guicheng Liu
Ni-rich cathodes are expected to serve as critical materials for high-energy lithium-ion batteries. Increasing the Ni content can effectively improve the energy density but usually leads to more complex synthesis conditions, thus limiting its development. In this work, a simple one-step solid-state process for synthesizing Ni-rich ternary cathode materials NCA (LiNi0.9Co0.05Al0.05O2) was presented, and the synthesis conditions were systematically studied. It was found that the synthesis conditions have a substantial impact on electrochemical performance. Furthermore, the cathode materials produced through a one-step solid-state process exhibited excellent cycling stability, maintaining 97.2% of their capacity after 100 cycles at a rate of 1 C. The results show that a one-step solid-state method can successfully synthesize Ni-rich ternary cathode material, which has great potential for application. Optimizing the synthesis conditions also provides valuable ideas for the commercial synthesis of Ni-rich cathode materials.Keywords:lithium-ion batteries;Ni-rich cathode materials;one-step solid-state synthesis;electrochemical performance
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高影响因子
MOLECULES
·
2023
·Vol. 28
·期 8
·3344
·
IF 4.6
Han Rao,Weiping Li,Fuzhen Zhao,Yongfa Song,Huicong Liu,Liqun Zhu,Haining Chen
In order to increase the hardness, wear resistance and corrosion resistance of nickel-based coatings, pure nickel is often co-electrodeposited with silicon carbide (SiC) particles. However, SiC particles tend to agglomerate and precipitate in the bath, which reduces the amounts of nanoparticles and causes nonuniformity. Herein, we solve these problems by using binary non-ionic surfactants (Span 80 and Tween 60) to effectively disperse SiC particles (binary-SiC) in the bath, which suppresses nanoparticles agglomeration and leads to uniformly distributed SiC particles in the composite coatings. In comparison to the Ni/SiC coatings electrodeposited from the commonly used SDS-modified SiC, the coatings prepared with binary-SiC (Ni/binary-SiC) show finer crystallization and a smoother surface. In addition, the Ni/binary-SiC coatings exhibit higher hardness (556 Hv) and wear resistance (2.95 mg cm−2). Furthermore, higher corrosion resistance is also achieved by the Ni/binary-SiC coatings.Keywords:Ni/SiC composite coatings;co-electrodeposition;binary non-ionic surfactants;nanoparticle agglomeration;wear resistance
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Mengyao Liu,Taotao Gao,Hongmei Li,Bo Xie,Chunqiong Hu,Yong Guo,Dan Xiao
Based on the incidence of diabetes, developing glucose sensors of superior performance with low-cost transition metals (TMs) has been the direction of many researchers, amorphous TMs with highly efficient electrocatalytic properties have attracted our interest. On this basis, amorphous nickel–cobalt bimetallic N -doped carbon nanoparticles on carbon cloth (a-Ni 2 /Co 1 -NC/CC) were fabricated from ZIF-8, which was then used to fabricate an enzyme-free glucose sensor. It was found that the a-Ni 2 /Co 1 -NC/CC had the best response to glucose in 0.4 M NaOH at 0.55 V (vs Hg/HgO). As compared to crystal Ni 2 /Co 1 nanoparticle on carbon cloth (c-Ni 2 /Co 1 NPs/CC), cyclic voltammetry (CV) and chronoamperometry studies revealed that the a-Ni 2 /Co 1 -NC/CC showed a significant increase in the efficient of electrochemical oxidation of glucose under optimal conditions, exhibiting a high sensitivity of 2.455 mA mM −1 cm −2 with a low detection limit of 0.15 μM (S/N = 3). Furthermore, the constructed sensor based on a-Ni 2 /Co 1 -NC/CC also has long-term stability and can be used to detect glucose accurately in beverages (pure milk, coffee drinks, tea drinks, and soda water) with reasonable recovery from 95.6 % to 105.6 %. This study provides a simple and feasible method for the construction of a highly sensitive non-enzyme glucose electrochemical sensor based on amorphous TMs.
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高影响因子
JOURNAL OF MATERIALS RESEARCH
·
2023
·Vol. 38
·期 9
·2359-2368
·
IF 2.7
Ma Junjie,Liu Hangcheng,Tao Zeyu,Liu Jianfeng,Yuan Binxia,Pan Weiguo,Shi Zhengrong
In order to reveal the relationship between the structure and the electrochemical oxygen reduction reaction (ORR) activity of different double transition metal decorated catalysts, three different double transition metal and N co-doped carbon material cathode catalyst materials (FeCo–NC, FeNi–NC and CoNi–NC) were prepared in this study. The FeCo–NC catalysts synthesised in this study still showed high ORR activity under alkaline conditions, with a half-wave potential of 0.783 V RHE , a mass activity (MA) of 11.36 A/g (0.77 V RHE ) and an ultimate current density of − 4.46 mA cm −2 ; after 30,000 cycles, the half-wave potential only decreased to 99.3% of the initial potential. Meanwhile, we employ MS to establish three different double transition metal and N co-doped graphene catalysts and to calculate and analyse their desorption properties, leading to the FeCo–NC material being the model with the highest ORR activity, which is consistent with the experimental results. Graphical Abstract
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Hui Wang,Hongyuan Chuai,Xiaoyi Chen,Jianlong Lin,Sheng Zhang,Xinbin Ma
Single-atom catalysts within M-N-C structures are efficient for electrochemical CO2 reduction. However, most of them are powdered and require a coating process to load on the electrode. Herein, we developed a facile approach to the synthesis of large-scale self-supported porous carbon nanofiber electrodes directly decorated with atomically dispersed nickel active sites using facile electrospinning, where poly(methyl methacrylate) was employed to tune well the distributions of pores located in carbon nanofibers. The above self-supported carbon nanofibers were applied as a gas diffusion electrode to achieve 94.3% CO Faraday efficiency and 170 mA cm–2 current density, which can be attributed to the effects of rich mesoporous structures favorable for adsorption and mass transfer of CO2 and single nickel catalysts effectively converting CO2 to CO. This work provides an efficient strategy to fabricate self-supported electrodes and may accelerate the progress toward industrial applications of single-atom catalysts in the field of CO2 electroreduction.
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