Journal of Energy Chemistry
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2020
·
IF 7.216
Shuangxi Lin,Ziwen Hao,Jindong Shen,Xiao Chang,Shouying Huang,Maoshuai Li,Xinbin Ma
The metal-support interaction is of critical importance to enhance the catalytic activity and selectivity. However, it is still challenging to construct an appropriate interaction starting from the catalyst fabrication and/or activation. We herein established low-temperature treatment of Ni 2+ ions impregnated on ceria in reductive atmosphere and reduction–oxidation cycles as effective approachs to regulate the metal-support interaction and raise the catalytic performance in the CO 2 methanation. The proposed construction approach yielded Ni/CeO 2 that displayed highly dispersed Ni nanoparticles in contact with CeO 2 (111) and (100) facet, higher density of surface oxygen vacancies and larger amounts of weak basic sites relative to the reference samples, which increased the capacity for H 2 and CO 2 adsorption/activation. The interaction resulted in appreciably (2–3 fold) higher activity in the CO 2 methanation with maintaining almost full selectivity to CH 4 and high stability. Coverage of Ni surface by CeO 2− x thin layer as a typical structure of strong metal-support interaction resulting from high-temperature reduction, can be alleviated via reduction–oxidation cycles. We also demonstrate the activation treatment-determined metal-support interaction effect can generally extend to (TiO 2 and ZrO 2 ) supported Ni catalysts.
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KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2020
·Vol. 37
·期 12
·2143-2151
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IF 2.69
Shi Guangyu,Wang Yuanhao,Cao Yafeng,Cai Weijie,Tan Fengzhi
A Ni/Ce 0.8 Zr 0.2 O 2 catalyst (NiCeZr-N) was synthesized by a facile co-nanocasting technique for syngas production from ethanol dry reforming. In addition, a series of characterization techniques, such as transmission electron microscopy (TEM), X-ray diffraction (XRD), inductive coupled plasma Emission Spectrometer (ICP), X-ray photoelectron spectroscopy (XPS), Raman and hydrogen temperature programmed reduction (H 2 -TPR) were selected to evaluate the physicochemical features of the as-prepared catalysts. Indeed, the results indicated that NiCeZr-N catalyst prepared by co-nanocasting method had a smaller particle size (<5 nm), relatively higher specific surface area (39 m 2 /g) and stronger metal-support interaction in comparison with another model catalyst obtained from conventional co-precipitation method (NiCeZr-P). Expectedly, these positive factors enabled NiCeZr-N catalyst to exhibit better activity and stability. Typically, ethanol is completely converted by using NiCeZr-N as catalyst and heating to 700 °C, and CO 2 conversion was as high as 65.3%. Interestingly, H 2 /CO was close to 1.1 at 650 °C, which could be used as feedstocks of Fischer-Tropsch process. Particularly, no obvious fluctuation of ethanol conversion and the product selectivity was observed during 40 h time-on-stream stability test.
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CELLULOSE
·
2020
·Vol. 27
·期 13
·7591-7605
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IF 4.21
Wang Haiyong,Hu Xiaohong,Liu Siwei,Cai Chiliu,Zhu Changhui,Xin Haosheng,Xiu Zhongxun,Wang Chenguang,Liu Qiying,Zhang Qi,Zhang Xinghua,Ma Longlong
The bi-functional Ni–W@C catalysts were prepared by one-pot reduction–carbonization method and used in hydrogenolysis of cellulose as well as raw lignocellulosic biomass to chemicals. The catalytic performance for cellulose conversion showed that it was more favorable for ethylene glycol (EG) production, obtaining the highest EG yield 60.1% over the Ni–W@C 700 catalyst. The Ni–W@C bimetallic catalysts are systematically characterized with BET, XRD, Raman, XPS, TEM techniques and experiments to probe the active catalytic sites of the catalysts. The effects of calcination temperature of Ni–W catalysts, reaction time, temperature and H 2 pressure on cellulose hydrogenolysis were investigated in detail. The Ni particles could lead to produce more W 5+ active sites, which promotes the glucose retro-aldol condensation to break the target C–C bonds. Metallic Ni catalyzed C=O hydrogenation and C–C hydrogenolysis, which could also avoid the coke formation. The EG selectivity was dependent on the synergy of WO x and Ni metal sites. In addition, this synergistic effect between the metal and WO x could promote lignin component degradation in direct conversion of untreated raw lignocellulosic biomass, obtaining the propyl monophenolics including guaiacylpropane, syringylpropane and p-n-propylphenol with a total yield of 17.3 wt% besides EG.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2020
·Vol. 27
·期 18
·22639-22647
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IF 3.056
Ren Qiangqiang,He Limo,Hu Song,Li Hanjian,Li Shanxue,Deng Zengtong,Song Gongxiang,Su Sheng,Wang Yi,Xiang Jun
The formation of highly graphitic phenolic resin chars (GPFCs) during catalytic carbonization at relatively low reaction temperature (1200–1600 °C) using novel Ni-Zn-B alloy catalyst with small amount of addition (5–15%) was systematically studied. Only two kinds of graphites (turbostratic graphite and ordered graphite) can be found in GPFCs after catalytic carbonization with Ni-Zn-B and their proportions were changed with reaction conditions. When Ni-Zn-B was involved at 1200–1600 °C, the phenolic resin char was fully transformed to be graphite, and ordered graphite content increased to 28.42% at 1400 °C, which was also almost twice of ordered graphite content in the char catalyzed by pure Ni. But the order graphite content would decrease due to sintering at higher reaction temperature. The addition of Zn and B can promote nickel-based alloy catalytic action by reducing melt point and accelerating graphitization respectively. It was also found that ordered graphite content could be used as a key evaluation parameter to directly reflect the quality of GPFCs based on detailed characteristics analysis. The model between three reaction conditions (reaction temperature, retention time, catalyst content) and ordered graphite content was built with artificial neural network (ANN), and the prediction accuracy of ANN was high up to 91.48%.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Lingjiao Li,Jing Xu,Binyi Su
In the field of photocatalysis, most of the photocatalysts are semiconductors. Recent years, there have been many photocatalytic systems related to non-semiconductor catalysts. In this paper, a photocatalytic hydrogen evolution system of hexagonal Ni(OH) 2 derived from CuNi bimetal is obtained by classical hydrothermal method. The derived hexagonal Ni(OH) 2 can promote the separation of photogenerated electron-hole pairs and greatly improve the effect of photocatalytic hydrogen evolution. The electron-hole pair comes from the surface plasmon resonance (SPR) effect of Cu from CuNi composite. It is worth noting that photoluminescence spectra and photoelectrochemical experiments have confirmed that the CuNi-5 complex can effectively improve space charge separation. The results of linear scanning voltammetry show that the material has high current response characteristics. This system gives a practical solution for planning and synthesizing non-semiconductor catalysts with high photocatalytic activity.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Yutong Wang,Lun Pan,Yixin Chen,Guoqiang Shen,Li Wang,Xiangwen Zhang,Ji-Jun Zou
Ni-based alloys are considered as the efficient catalyst for hydrogen-storage materials decomposition. Herein, we applied an in-situ melt-quenching method to dope Mo in Ni-based alloy for catalytic hydrogen evolution from hydrogen-storage materials. Importantly, Mo doped Ni-based catalyst exhibits more than 6 times higher TOF value than that of pure Ni both in AB hydrolysis and hydrazine decomposition, because Mo acts as an electron donor to improve the reducibility of Ni. Hydrogen evolution kinetics were studied over a range of temperatures (303–353 K) and initial feed concentrations (catalyst/hydrogen-storage materials (wt/wt) ratios = 0.2–10). Under optimal reaction conditions, the H 2 evolution rate reaches 1.92 mol H 2 /(mol cat min) and 0.05 mol H 2 /(mol cat min) in the hydrolysis of ammonia borane and decomposition of hydrazine, which are 6.42 and 6.44 times higher than undoped Ni catalyst, respectively. And the apparent activation energy of ammonia borane hydrolysis and hydrazine decomposition were evaluated to be 26.66 ± 3.31 kJ/mol and 40.01 ± 3.38 kJ/mol, respectively.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
·
IF 7.489
Hao Gu,Qin Zhong,Yiqing Zeng,Shule Zhang,Yunfei Bu
The supercapacitive performance of high-rate capacity and long-term cycling stability is still a big challenge for electroactive materials. Herein, Ni and Zn co-substituted Co carbonate hydroxide (NiZn-CoCH) flowers array is self-assembled on nickel foams (NFs) using l -ascorbic acid as a nanostructure inducer. The NiZn-CoCH flowers, consisting of silk-like nanosheets, are deservedly large electrode-electrolyte contact area and suitable ion-diffusion channel. The nanostructure and Ni and Zn co-substitution significantly improve energy storage performance. This electrode exhibits a high specific capacitance of 2020.8 F g −1 at 1 A g −1 with high-rate capacity (remain 80.2% at 10 A g −1 ) and 5000-cycle stability (almost unchanged after 1500 cycles at 10 A g −1 ). Additionally, an assembled asymmetric supercapacitor (ASC) device of NiZn-CoCH//activated carbon (AC) achieves a high energy density of 29.6 Wh kg −1 at a power density of 375 W kg −1 and only a 0.5% decrease of the capacitance after 2500 cycles. This facile and novel preparation method, using l -ascorbic acid, may be promising for industrial production of electroactive materials for the high-performance energy storage and conversion devices.
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高影响因子
HYDROMETALLURGY
·
2020
·
IF 3.338
Xintao Yi,Guangsheng Huo,Wei Tang
The extraction of Fe(III), Ni(II) and Co(II) from a Ni(II)-Co(II) solution containing Fe(III) was analyzed in a chloride medium using a mixed extractant consisting of 50% ( v /v) tributyl phosphate (TBP), 20% (v/v) 2-octanol and 30% (v/v) kerosene. The extraction of 0.5 mol/L Fe(III) in 4 mol/L hydrochloric acid reached 97%, and the consumption of chloride ions was investigated. Nickel(II) ions were not detectably extracted by TBP, with an inclusion of <1.1%. Compared with Fe(III), TBP extracted only a small amount of Co(II). The iron complexes formed by TBP and 2-octanol were [H 2 FeCl 4 · 2TBP] and [H 2 FeCl 4 · 5(2-octanol)], and the possible compositions of Co-containing extracts were [H 2 CoCl 4 · 2TBP] and [H 2 CoCl 4 ] · n[2-octanol]. An industrial process consisting of two-step extraction was designed to achieve the separation of Co(II) and Fe(III), resulting in a decrease in the Fe/Co mass ratio from 0.46 to <3.5 × 10 −4 in the raffinate.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
·
IF 7.489
Linhua Rao,Jiayi Tang,Sufei Hu,Liguo Shen,Yanchao Xu,Renjie Li,Hongjun Lin
While electroless nickel plating is considered as a promising candidate for fabrication of metallized polymer composite membranes with high performance, it suffers from problems of complex and high-cost pretreatment procedure, hindering its large-scale implementations. It is hypothesized that, inkjet printing integrated with electroless plating (ELP) can serve as a facile and economical membrane fabrication method to overcome above problems. The new method proposed in this study was processed by inkjet printing silver ions and pyrrole inks as catalytic layer followed by electroless Ni deposition on polypropylene (PP) membrane surface. Successful modification was verified by characterizing the surface morphology and elemental compositions of the membranes. In comparison to the pristine PP membrane, the PPy-Ag/Ni modified membrane demonstrated lower surface resistance (2.3 Ω), better hydrophilicity (44.9°) and higher pure water flux (1135.1 L m −2 h −1 ). When applying an external electric field (10.0 V cm −1 ), the average flux of the PPy-Ag/Ni membrane for yeast filtration increased from 107.8 to 137.7 L m −2 h −1 , which was about 2.0 times higher than that of the pristine PP membrane. Meanwhile, the PPy-Ag/Ni membrane possessed a maximum flux recover rate when applied with an external electrical field. This work provided a facile and efficient approach for fabrication of composite conductive membranes.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 6
·064513
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IF 4.316
Yunyi Xu,Wen Jin,Tingting Yu,Feng Wang,Xiaoyu Guo,Yiping Wu,Ye Ying,Ying Wen,Haifeng Yang
The development of durable and efficient anode electrocatalysts is crucial for direct methanol fuel cells. In this paper, polyaniline (PANI) microtubes are firstly prepared by removing the polystylene (PS) core from PANI coated electrospun PS. The catalyst of PtNi/PANI@rGO is built by two steps: graphene oxide (GO) is mixed with PANI microtubes to obtain PANI@GO and then PANI@GO is used as a support material to load PtNi nanoparticles by reductive reaction while GO is reduced into rGO. The morphology, electronic structure and chemical structure of the catalysts are characterized by SEM, TEM, XPS and Raman spectroscopy, respectively. The electrochemical analysis of electrochemical impedance spectroscopy, cyclic voltammetry and chronoamperometric measurement are performed to analyze the electrocatalytic performance. The electrochemical results indicate that as-synthesized PtNi/PANI@rGO has the high activity toward methanol oxidation, and its mass activity is 1.7, 1.3 and 4.1 times higher than that of PtNi/PANI, PtNi/rGO and commercial Pt/C catalysts, respectively. The PANI microtubes not only improve the electron transfer kinetic but also help avoid the accumulation of graphene layers. The doping of Ni into Pt changes the surface electronic structure to elevate the catalytic activity and helps effectively improve the resistance to CO poisoning.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Guojuan Hai,Jianfeng Huang,Liyun Cao,Koji Kajiyoshi,Long Wang,Liangliang Feng,Jun Chen
The electrochemical conversion is closely correlated with the electrocatalytic activities of the electrocatalyst. Herein, the urchin-like Ni-doped W 18 O 49 /NF with enriched active sites was prepared by solvothermal method followed by a low-temperature pyrolysis treatment was reported. Results demonstrate that the incorporation of Ni-doping triggers the lattice distortion of W 18 O 49 for the increasement of oxygen defects. Further, high-valent W 6+ are partially reduced to low-valent W 4+ , wherein the electrons originate from the oxidation process of Ni 2+ to Ni 3+ . The Ni 3+ ions show an enhanced orbital overlap with the OER reaction intermediates. The generated W 4+ ions contribute to release oxygen vacancies, eventually reorganizing Ni-doped W 18 O 49 /NF to unique electrochemical active species with a special amorphous-crystalline interface (AM/NiWO x /NiOOH/NF). Simultaneously, the reconstruction results in an optimized valence band and conduction band. Eventually, the resultant AM/NiWO x /NiOOH/NF with abundant active sites and improved oxidation/reduction capability exhibits more superior catalytic performance compared with the Ni-doped W 18 O 49 /NF counterpart. This study gives more insights in the electrochemical evolution of the tungsten-based oxide and provides effective strategies for optimizing the catalytic activity of materials with inherent hydrogen evolution reaction limitations.
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CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Dongdong Wang,Wanbing Gong,Jifang Zhang,Miaomiao Han,Chun Chen,Yunxia Zhang,Guozhong Wang,Haimin Zhang,Huijun Zhao
Catalytic hydrodeoxygenation (HDO) is one of the most promising strategies to transform oxygen-rich biomass derivatives into high value-added chemicals and fuels, but highly challenging due to the lack of highly efficient nonprecious metal catalysts. Herein, we report for the first time of a facile synthetic approach to controllably fabricate well-defined Ni-Co alloy NPs confined on the tip of N-CNTs as HDO catalyst. The resultant Ni-Co alloy catalyst possesses outstanding HDO performance towards biomass-derived vanillin into 2-methoxy-4-methylphenol in water with 100% conversion efficiency and selectivity under mild reaction conditions, surpassing the reported high performance nonprecious HDO catalysts. Impressively, our experimental results also unveil that the Ni-Co alloy catalyst can be generically applied to catalyze HDO of vanillin derivatives and other aromatic aldehydes in water with 100% conversion efficiency and over 90% selectivity. Importantly, our DFT calculations and experimental results confirm that the achieved outstanding HDO catalytic performance is due to the greatly promoted selective adsorption and activation of C=O, and desorption of the activated hydrogen species by the synergism of the alloyed Ni-Co NPs . The findings of this work affords a new strategy to design and develop efficient transition metal-based catalysts for HDO reactions in water.
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