ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Pengfei Shang,Zhiguo Ye,Yi Ding,Zhixiang Zhu,Xinyuan Peng,Guang Ma,Duosheng Li
Owing to unstable electrical energy generation from intermittent solar and wind energy sources, the development of efficient and durable nonnoble electrocatalysts is extremely desirable, in particular, those that can be used over a wide range of current densities for the hydrogen evolution reaction (HER), especially >1 A cm–2, which is extremely desirable for energy transformation in power systems. Here, a nanosponge-like NiMo solid solution based on a nanoscale Kirkendall effect is fabricated via a one-step high-temperature sintering method. A polycrystalline layer of NiMo oxyhydroxide is formed on the surface of the as-prepared electrode after aging, thus achieving a low overpotential and Tafel slope of 37 mV at 10 mA cm–2 and 39.2 mV dec–1, respectively. The electrode displays superior electrochemical stability over a wide range of current densities without compromising its electrocatalytic activity; in particular, it is durable for over 300 h at 2 A cm–2. This is attributed to the combination of the 3D-interconnected nanosponge structure, synergistic effect between the Ni and Mo species, lattice distortion of the solid solution, and its high conductivity. This work provides a possible commercialization for the fabrication of nonprecious electrocatalysts with high performance in large-scale energy conversion.
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ACS Applied Materials & Interfaces
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2020
·
IF 8.758
Guangfu Qian,Jinli Chen,Lin Luo,Hao Zhang,Wei Chen,Zhejiang Gao,Shibin Yin,Panagiotis Tsiakaras
Developing high performance bifunctional transition metal catalysts would be significantly beneficial for electrocatalytic oxidation of urea-rich wastewater. Herein, we synthesize a V2O3 nanosheet anchored N-doped-carbon encapsulated Ni heterostructure (Ni@C–V2O3/NF) for the reactions of urea oxidation (UOR) and hydrogen evolution (HER). Electrochemical results indicate that it exhibits small potentials of 1.32, 1.39, and 1.43 V for UOR and low overpotentials of 36, 254, and 355 mV for HER at ±10, ± 500 and ±1000 mA cm–2, respectively. It can work at 100 mA cm–2 for over 72 h as cathode and anode electrode without obvious attenuation, suggesting an outstanding durability. The reason for this behavior could be ascribed to the N-doped-carbon coating structure, the synergetic effects between Ni and V2O3, and the nano/micro nanosheets architecture self-supported on nickel foam. This work could provide a promising, inexpensive, and green method for the degradation of urea-rich wastewater and hydrogen production.
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PubMed
高影响因子
Sustainable Energy & Fuels
·
2020
·Vol. 4
·期 4
·1883-1890
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IF 5.503
Chengbo Wei,Xiaoming Fan,Xue Deng,Linzheng Ma,Xiao Zhang,Qingyun Liu,Jinxue Guo
Efficiently generating hydrogen in neutral solution is essentially important for electrocatalysts toward practical application of water splitting; however, most of the catalysts show promising activity only in acidic or alkaline media. Herein, a surface modulation method is developed via doping Ru onto the surface of a Ni2P nanosheet array supported on nickel foam (Ru-Ni2P/NF) to activate the robust hydrogen evolution activity. The Ru species achieve optimized surface chemistry for catalysis, including boosted intrinsic activity, improved catalytic center density, and enhanced kinetics. The as-obtained electrode exhibits Pt-like catalytic activity, as well as good stability in both neutral and alkaline solution. Exploring efficient and wide-pH electrocatalysts by such surface chemistry modulation would be of great value for the development of advanced materials for energy conversion.
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Sustainable Energy & Fuels
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2020
·Vol. 4
·期 6
·2768-2774
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IF 5.503
Qinghai Yang,Congquan Zhou,Jihong Ni,Xiaofei Guan
We present a liquid catalytic system comprising a liquid Ni–Bi alloy and a molten K2CO3 salt, which completely resolves the coking and sintering issues for dry reforming. The conversions of CH4 and CO2 reach 60% and 70%, respectively, in a 30 cm bubble column comprising 15 cm Ni0.27Bi0.73 and 15 cm K2CO3 at 1050 °C. The CO selectivity is near 100% throughout the temperature range of 950–1050 °C. A 120 hour stability test at 1000 °C shows no performance degradation, suggesting a stable and effective dry reforming process for syngas production. The catalytic performance and durability demonstrated highlight the potential of dry reforming for commercial applications.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Shanshan Qiao,Chao Feng,Yuan Guo,Tingxiang Chen,Naeem Akram,Yi Zhang,Wei Wang,Fan Yue,Jide Wang
The exploration of bifunctional catalysts to produce both hydrogen and oxygen will accelerate the progress of overall water-splitting. This paper introduces a facile method to fabricate bifunctional photocatalysts toward the water splitting by doping nano CdS with S vacancies on Ni@NiO nano-spheres. A serious of photocatalytic catalysts were developed and subsequently characterized, the two half-reactions of photocatalytic water splitting were studied in detail by using sacrificial agents, the hydrogen output at 41699 μmol g −1 h −1 (AQE 28.5%, λ = 420 nm) while the evolution of O 2 is as high as 55120 μmol g −1 h −1 (AQE 35.7%, λ = 450 nm). It is a strategy that the presence of Ni@NiO can trigger the S vacancy in CdS to act as an effective electron trap, the p-n junction of NiO-CdS, as well as the Schottky barrier between NiO and Ni, can change the dynamic characteristics of photogenerated electrons and prolong their life. These prolonged photogenerated electrons can initiate stable and effective photocatalytic redox reactions.
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Journal of Materials Chemistry A
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2020
·Vol. 8
·期 11
·5699-5708
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IF 11.301
Xin Qian,Dongyang Wang,Yang Zhang,Haijun Wu,Stephen J. Pennycook,Lei Zheng,Pierre F. P. Poudeu,Li-Dong Zhao
The metallic elements with a small atomic radius can not only compensate for the intrinsic vacancies to improve the carrier mobility, but also can form interstitials to reduce lattice thermal conductivity. In this work, we investigate the contrasting roles of three different metallic elements with small atomic radius on the thermoelectric properties of n-type PbM0.01Se (M = Cu, Zn, Ni). We find that all the metallic elements can increase the carrier concentration as electron donors and improve the electrical transport properties. In addition, the lattice thermal conductivity of PbSe can be significantly decreased through the formation of interstitials by the incorporated extra metallic elements. We also find that the PbCu0.01Se sample exhibits a unique and complex behavior compared with the other samples due to the diffusion and the thermally activated oxidation of Cu+ ions. When the temperature increased to 673 K, the carrier concentration of PbCu0.01Se sample increases suddenly and continues to increase by nearly two folds, which we ascribe to the release of 3d orbital electrons in Cu+ ions. This results in a strong decoupling of the charge and heat transport in the material, which can be manifested by the overestimation of the electronic thermal conductivity when assuming strong electron–phonon coupling in Wiedemann–Franz law. A maximum ZT of ∼1.6 can be reached at 773 K and the average ZT of ∼0.96 can be achieved in PbCu0.01Se. Our results demonstrate the exceptional contrasting behavior of Cu in PbSe by comparing with Zn and Ni, and the thermoelectric performance of n-type PbSe can be enhanced through the introduction of extra metallic elements with small radius.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Yanpei Li,Xiangwei Wu,Jingyi Wang,Xingpeng Gao,Yingying Hu,Zhaoyin Wen
The sodium-nickel chloride (Na-NiCl 2 ) batteries technology has been considered as one of the most promising candidates for large-scale electrical energy storage application owing to its abundant electrode material resource, high energy density and safety. However, ultra-excessive Ni in the cathode leads to high material cost and the growth of cathode particles during cycles makes degradation of batteries performances, which hinder the further application of Na-NiCl 2 batteries. To address these challenges, we designed a free-standing Ni-less cathode with Ni/NaCl particles uniformly distributed in the three-dimensional (3D) conductive matrix constructed by carbonfiber (CF) and multiwalled carbon nanotubes (MWCNTs). The 3D hierarchical structure synthesized by low-cost vacuum filtration method can offer sufficient void space to accommodate the growth of NaCl particles and effectively enhance the electronic conductivity of the cathode. When the molar ratio of Ni/NaCl in the cathode is reduced to 1.0, a specific capacity of 90 mAh g −1 for planar Na-NiCl 2 batteries can be achieved after 170 cycles at 190 °C with a capacity retention of 67%, which is higher than that of traditional tubular Na-NiCl 2 batteries.
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JOURNAL OF THERMAL SPRAY TECHNOLOGY
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2020
·Vol. 29
·期 7
·1827-1837
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IF 2.522
Zhang Ying,Han Tengfei,Xiao Meng,Shen Yifu
The diamond enhanced (NiCoCrTi 0.5 Nb 0.5 )C x ( x = 3, 6, 12 wt.%) high-entropy alloy coatings were well-prepared by laser cladding, which are denoted as C 3 , C 6 and C 12 , respectively. The macroscopic morphology, phase, microstructure, hardness and wear resistance were investigated. The coatings without pores and cracks, are well-metallurgically bonded with the substrate. The width, melting depth and dilution rate of (NiCoCrTi 0.5 Nb 0.5 )C x coating decrease with the increase of diamond content. The coatings are mainly composed of BCC solid solution, (Ti,Nb)C and Cr 3 C 2 . The increase of diamond content results in the precipitation of (Ti,Nb)C and Cr 3 C 2 , and the coating with x = 12 wt.% retains more diamonds. The hardness of coatings is much higher than that of the substrate. As the diamond content increases, the average hardness of (NiCoCrTi 0.5 Nb 0.5 )C x coating increases first and then decreases. The abrasive wear occurs in each coating. The wear depth, roughness and wear rate decrease first and then increase as the diamond content increases. The C 6 coating with the better wear resistance produces a smooth worn surface, which indicates that C 6 coating can be fully applied to various tools, molds and mechanical parts.
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ACS Catalysis
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2020
·
IF 12.35
Haiyong Wang,Haosheng Xin,Chiliu Cai,Changhui Zhu,Zhongxun Xiu,Qiying Liu,Yujing Weng,Chenguang Wang,Xinghua Zhang,Shijun Liu,Zifang Peng,Longlong Ma
Keto-alcohols, which are traditionally produced from fossil resources with multisteps, are considered as important intermediates for diversified high-value-added fine chemical synthesis due to their involved carbonyl and hydroxyl groups. Herein, direct cellulose hydrogenolysis to C3-C4 keto-alcohol products (hydroxyacetone and 1(3)-hydroxy-2-butanone) was achieved over Ni-WOx/C catalysts with an W/Ni atom ratio of 1.0–5.0. The keto-alcohol yield was proposed to strongly depend on the W/Ni ratio and the catalyst annealing temperature. The highest keto-alcohol yield of 63% was obtained at the optimal balance of basic/acidic WOx species and metallic Ni. The introduction of Ni facilitated the formation of the basic W5+ sites, which enhanced the formation of basic sites at the Ni-WOx interface. The synergistic effect between the basic W5+ and acidic oxygen vacancy (Vö) could activate the target C–O/C═O bonds, promoting the isomerization of glucose and C3-C4 aldehyde intermediates with the assistance of the interfacial Ni. The cooperative adsorption of the −OH and −C═O groups at the Ni-O-W-Vö interface stabilized the adjacent ketone and hydroxyl groups and kept the other hydroxyl groups for hydrogenolysis, obtaining the final C3-C4 keto-alcohols. This work expanded the application of cellulosic biomass, enabling the green and sustainable synthesis of the high-value C3-C4 keto-alcohol products using lignocellulosic biomass as a raw material.
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Journal of Energy Chemistry
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2020
·
IF 7.216
Jia Sun,Lei Du,Baoyu Sun,Guokang Han,Yulin Ma,Jiajun Wang,Hua Huo,Pengjian Zuo,Chunyu Du,Geping Yin
ABO 3 -type perovskite oxides (e.g., LaCoO 3 ) with flexible and adjustable A- and B-sites are ideal model catalysts to unravel the relationship between the electronic structure and electrocatalytic activity (e.g., oxygen reduction/evolution reactions, ORR/OER). It has been well understood in our recent work that the secondary metal dopant at B-site (e.g., Mn in LaMn x Co 1 −x O 3 ) can regulate the electronic structure and improve the ORR/OER activity. In this work, the Mn-Ni pairs are employed as the dual dopant in LaMn x Ni y Co z O 3 ( x + y + z = 1) catalysts toward bifunctional ORR and OER. The structure–property relationships between the triple metal B-site (Mn, Ni and Co) and the electrochemical performance are particularly investigated. Compared to the individual Mn doping (e.g., LaMnCoO 3 (Mn:Co = 1:3) catalyst), the dual Mn-Ni doping significantly improves the ORR mass activity@0.8 V by 1.54 times; meanwhile, the OER overpotential@10 mA cm −2 is reduced from 420 to 370 mV, and the OER current density at 1.55 V is increased by 2.43 times. Reasonably, the potential gap between E ORR @-1 mA cm −2 and E OER @10 mA cm −2 is achieved as only 0.76 V by using the optimal LaMn x Ni y Co z O 3 ( x : y : z = 1:2:3) catalyst. It is revealed that the dual Mn-Ni dopant efficiently optimizes electron structures of the LaMnNiCoO 3 (1:2:3) catalyst, which not only decreases the e g orbital electron number, but also modulates the O 2p-band closer to the Femi level, accounting for the enhanced bifunctional activity.
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高影响因子
CELLULOSE
·
2020
·Vol. 27
·期 13
·7591-7605
·
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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SURFACE & COATINGS TECHNOLOGY
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2020
·
IF 3.784
Ying Zhang,Tengfei Han,Meng Xiao,Yifu Shen
(FeNiCoCrTi 0.5 )C x (x = 3 wt%, 6 wt%, 12 wt%) carbonized high-entropy alloy-based composite coatings , marked as C 3 , C 6 and C 12 , were prepared on 45 steel by laser cladding. The macroscopic morphology, phase, microstructure, hardness and wear resistance of coatings have been investigated systematically. The results indicate that diamond content has a significant influence on the microstructure and mechanical properties of (FeNiCoCrTi 0.5 )C x coating. (FeNiCoCrTi 0.5 )C x coatings, without pores and cracks, are well metallurgically bonded with substrate. The coatings consist of BCC solid solution, Cr 23 C 6 and TiC. The addition of diamond in (FeNiCoCrTi 0.5 )C x coating leads to the instability of BCC solid solution and facilitates the precipitation of carbides , which causes carbides to become coarse and aggregate into large blocks. The hardness of (FeNiCoCrTi 0.5 )C x coatings is much higher than that of the 45 steel, the average hardness of C 12 coating is 4 times the hardness of substrate. Besides, the hardness of (FeNiCoCrTi 0.5 )C x coating increases with the increase of diamond content. Nonetheless, compared to C 6 coating, the C 12 coating shows inferior tribological performance due to the brittleness . It is noteworthy that C 6 coating with outstanding wear resistance has the potential to apply in various fields of machinery industry, marine engineering and aerospace.
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