CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Zekai Mu,Xianglei Liu,Hang Shi,Chao Song,Chunzhuo Dang,Ke Gao,Nan Sun,Cheng Tian,Hangbin Zheng,Xinrui Wang,Yimin Xuan
By converting two greenhouse gases into fuels, CO 2 reforming of CH 4 via free and clean solar energy is a promising solution to the energy shortage and global warming problems simultaneously. However, serious challenges such as limited light-to-fuel efficiency, severe catalyst aggregation, and deactivation still exist for reactors employing traditional catalyst powders. Here, Ni/MgAlO x -LDH catalysts loaded Ni foam reactor with heat recovery is proposed for highly efficient and stable CO 2 reforming under direct concentrated solar irradiation. The temperature nonuniformity is reduced by 84.3% compared to powdered systems, which benefits from the high thermal conductivity of nickel foams. Overheating is also prevented, which leads to much less carbon deposition and relieved active sites aggregation. Ultrahigh light-to-fuel efficiency of 36.51% is achieved, which is much higher than that of traditional powdered systems (23.87%). Numerical simulation results have an excellent agreement with experiments and demonstrate that heat recovery can greatly improve CRM rates by 23.8%. This work opens new routes to achieve highly efficient, stable, and scalable solar-driven CO 2 reforming via Ni/MgAlO x -LDH catalysts loaded Ni foam reactors with heat recovery.
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FUEL
·
2020
·
IF 5.578
Limo He,Song Hu,Xiaofei Yin,Jun Xu,Hengda Han,Hanjian Li,Qiangqiang Ren,Sheng Su,Yi Wang,Jun Xiang
Fe-modified Ni/Al 2 O 3 catalysts with Fe/Ni molar ratios of 0, 0.5, 1 and 2 were prepared to promote the co-production of H 2 and carbon nanotubes (CNTs) during steam reforming of toluene as a tar model compound. After the addition of Fe, toluene conversion increased from 55.1% of Ni/Al 2 O 3 to 73.6% of F1N1A (Fe/Ni ratio of 1), and H 2 yield over F1N1A reached the maximum of more than 2000 mmol/(g-cata). Multi-walled carbon nanotubes with average diameter of 10–30 nm were generated and follow tip-growth mechanism. Compared with Ni/Al 2 O 3 , the addition of Fe remarkably increased the amount and quality of CNTs which had longer length and less tortuosity. These dual promoting effects on H 2 and CNTs after the addition of Fe were attributed to the strong interaction between Ni and Fe in Fe-Ni alloy. Fe-Ni alloy had the high activity for the decomposition performance of toluene and H 2 O to generate more H 2 and intermediates for improving the reforming reaction. Meanwhile, the high catalytic decomposition activity supplied more carbon species and the formation of Fe-Ni alloy enhanced the generation of metal carbide for promoting CNTs growth. Besides, the deposition of amorphous carbon was suppressed and the interaction between Ni particle and catalyst support was weakened after the addition of Fe, which kept the activity of catalyst and promoted the tip-growth of CNTs.
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CHEMOSPHERE
·
2019
·
IF 5.108
Xin Ning,Yuhan Sun,Heyun Fu,Xiaolei Qu,Zhaoyi Xu,Shourong Zheng
Metal-organic frameworks (MOFs) have received significant attention as promising precursors or sacrificial templates in the preparation of porous carbon supported catalysts. In this study, N-doped porous carbon supported Ni catalysts (denoted as Ni/NC) were prepared using furfuryl alcohol (FA) loaded Ni-MOF-74 as the precursor followed by NH 4 OH treatment and pyrolysis under N 2 atmosphere. For comparison purpose, Ni catalysts supported on porous carbon (denoted as Ni/C) were also prepared by direct pyrolysis of Ni-MOF-74. The selective gas phase catalytic hydrodechlorination of 1,2-dichloroethane to ethylene was carried out to evaluate the catalytic performances of the catalysts. It was found that for Ni catalysts prepared at the same pyrolysis temperature, Ni particle sizes in Ni/NC catalysts were significantly smaller (20–40% smaller) than that of Ni/C. This reflected that pre-modification of Ni-MOF-74 using FA and NH 4 OH could effectively increase Ni dispersion in Ni catalysts derived from Ni-MOF-74. Moreover, Ni/NC had a markedly stronger ability to form spillover H 2 owing to the enhanced metal-support interactions by N-doping. Accordingly, Ni/NC catalysts exhibited much higher catalytic activities than Ni/C catalysts. The turnover frequencies of Ni/NC catalysts were found to be 1.22–1.65 times higher than Ni/C catalysts. Increasing pyrolysis temperature led to decreased catalytic activities of both Ni/C and Ni/NC catalysts, due to the aggregation of Ni particles at higher treatment temperature. The findings from this study demonstrate that the MOF-mediated synthesis method offers a promising way to prepare Ni-based catalysts for catalytic hydrodechlorination of chlorinated hydrocarbons .
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Guangxin Ren,Baocang Liu,Liang Liu,Minghao Hu,Junpeng Zhu,Xuan Xu,Peng Jing,Jinfang Wu,Jun Zhang
Biomass is a sustainable and renewable resource that can be converted into valuable chemicals, reducing the demand for fossil energy. 5-Hydroxymethylfurfural (HMF), as an important biomass platform molecule, can be converted to high-value-added 2,5-furandicarboxylic acid (FDCA) via a green and renewable electrocatalytic oxidation route under mild reaction conditions, but efficient electrocatalysts are still lacking. Herein, we rationally fabricate a novel self-supported electrocatalyst of core–shell-structured copper hydroxide nanowires@cerium-doped nickel hydroxide nanosheets composite nanowires on a copper mesh (CuH_NWs@Ce:NiH_NSs/Cu) for electrocatalytically oxidizing HMF to FDCA. The integrated configuration of composite nanowires with rich interstitial spaces between them facilitates fast mass/electron transfer, improved conductivity, and complete exposure of active sites. The doping of Ce ions in nickel hydroxide nanosheets (NiH_NSs) and the coupling of copper hydroxide nanowires (CuH_NWs) regulate the electronic structure of the Ni active sites and optimize the adsorption strength of the active sites to the reactant, meanwhile promoting the generation of strong oxidation agents of Ni3+ species, thereby resulting in improved electrocatalytic activity. Consequently, the optimal CuH_NWs@Ce:NiH_NSs/Cu electrocatalyst is able to achieve a HMF conversion of 98.5% with a FDCA yield of 97.9% and a Faradaic efficiency of 98.0% at a low constant potential of 1.45 V versus reversible hydrogen electrode. Meanwhile, no activity attenuation can be found after 15 successive cycling tests. Such electrocatalytic performance suppresses most of the reported Cu-based and Ni-based electrocatalysts. This work highlights the importance of structure and doping engineering strategies for the rational fabrication of high-performance electrocatalysts for biomass upgrading.
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JOURNAL OF ELECTRONIC MATERIALS
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2024
·
IF 2.2
Hou Guangya,Wu Yitao,Chen Qiang,Zhang Jianli,Tang Yiping
Constructing low-cost, high-catalytic-performance anode electrocatalysts is a significant challenge for methanol oxidation (MOR) and urea oxidation (UOR) reactions. Using paper templates with abundant pores to prepare thin porous metal materials helps to obtain high-performance electrode materials. The nano amorphous B-doped Ni/crystalline Ni (nanoam Ni-B/Ni) foil composite electrodes were derived from paper templates prepared by impregnation, high-temperature reduction, and electrodeposition methods. Porous Ni foils (Nip) derived thinnest rice (“Xuan”) paper, initially used for Chinese calligraphy and painting, exhibits the best performance due to its strong adsorption and wettability. Compared to direct current electrodeposition, pulse electrodeposition yields finer amorphous B-doped Ni nanoparticles with good catalytic performance. Under a current density of 100 mA·cm −2 , the nanoam Ni-B/Ni composite electrode prepared under a duty cycle of 0.5–1.0 s achieved current densities of 290.4 mA·cm −2 (MOR) and 340.4 mA·cm −2 (UOR) at 0.8 V, which are improved by 37.1% and 55.1%, respectively, compared to those of Nip. After 2000 cycles, with solution replacement, the current densities maintained 99.2% (MOR) and 81.6% (UOR) of the original values, showing excellent electrocatalytic stability. This research provided a new use for Chinese rice paper, and the prepared Nip-based electrode, with a thickness of about 60 μm and a low area quality, had a simple preparation process and good electrochemical properties, and can be used as a potential substitute for commercial Ni foam for portable or small electrochemical devices. Graphical Abstract
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Yang Xiang,Linjian Yu,Kun Xiong,Haidong Zhang,Jia Chen,Xueqing Shi,Min Deng,Shiqian She
Using urea oxidation reaction (UOR) instead of oxygen evolution reaction (OER) is one of promising strategies for significantly diminish power consumption for hydrogen production from electrochemical water splitting. The electrocatalysts with cost-effective, multifunctional and high-performance are urgently required for enhancing UOR and hydrogen evolution reaction (HER), but this remains a challenge. Herein, we designed a bifunctional Ni(OH) x /p-Ni catalyst by electrochemical oxidation of Ni(OH) 2 in-situ grown on the surface of porous Ni membrane (p-Ni) to generate more abundant high-valence Ni 3+ active species, which is favorable for reducing the energy barrier of electrochemical reaction . At the same time, a large number of metallic oxygen bonds (Ni–O) were formed to optimize the reaction kinetics of the electrochemical process, thus promoting the overall urea electrolysis efficiency. In 1.0 M KOH with 0.3 M urea, the optimized Ni(OH) x /p-Ni only requires potentials of 1.38 V and 0.22 V to obtain a current density of 100 mA cm −2 for UOR and HER, respectively. Notably, by assembling the Ni(OH) x /p-Ni as the cathode and anode for hydrogen production from urea-assisted water splitting, it can drive a current density of 100 mA cm −2 at a low voltage of 1.52 V and has excellent stability. This work provides a feasible strategy for design efficiently non-noble metal electrocatalysts for energy-saving hydrogen production and purifying urea-rich wastewater.
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MOLECULES
·
2025
·Vol. 30
·期 4
·820
·
IF 4.6
Huijuan Han,Yalei Zhang,Chunrui Zhou,Haixin Yun,Yiwen Kang,Kexin Du,Jianying Wang,Shujun Chao,Jichao Wang
To achieve the “double carbon” goal, it is urgent to reform the energy system. The oxygen evolution reaction (OER) is a vital semi-reaction for many new energy-storage and conversion devices. Metal nanoparticles embedded in heteroatom-doped carbon materials prepared by the pyrolyzing of metal–organic frameworks (MOFs) have been a key route to obtain high-performance electrochemical catalysts. Herein, a nanocatalyst embedding Ni nanoparticles into S- and N-co-doped carbon nanoplate (Ni NPs@SN-CNP) has been synthesized by pyrolysis of a Ni-MOF precursor. The prepared Ni NPs@SN-CNP exhibits superior oxygen evolution performance with an overpotential of 256 mV to attain 10 mA cm −2 and a low Tafel slope value of 95 mV dec −1 . Moreover, a self-assembled overall-water-splitting cell with Ni NPs@SN-CNP/NF||Pt-C/NF achieves a low potential of 1.56 V at 10 mA cm −2 and a high cycling stability for at least 10 h. The improvement in this performance is benefit from its large surface area, unique morphology, and the nanostructure of the electrocatalyst. This study presents a novel and simple approach to designing high-performance OER catalysts.
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Nanoscale
·
2019
·Vol. 11
·期 19
·9598-9607
·
IF 6.97
Shiyu Zhang,Zhendong Yang,Ke Gong,Ben Xu,Hao Mei,Haobing Zhang,Jiaxin Zhang,Zixi Kang,Youguo Yan,Daofeng Sun
Conformal hydrolysis of MOF precursors is a promising strategy to prepare hierarchical metal hydroxide electrode materials on a large scale with low cost and high efficiency. However, a complete transformation is challenging due to the normal “outside-in” conversion process. After studying the hydrolysis of Ni-MOF-74, which has regular 1D channels, we suggest that the transformation to Ni(OH)2 can occur simultaneously outside and within the precursor depending on the treatment temperature. Molecular dynamics simulations reveal that a higher temperature weakens the steric effects of OH− ions and facilitates the diffusion in the regular channels, and therefore, a complete transformation from Ni-MOF-74 to Ni(OH)2 is achieved. It is for the first time demonstrated that the 1D channels of MOFs are utilized for the complete conformal hydrolysis of Ni-MOF-74 to Ni(OH)2 electrode materials. Meanwhile, we also perform pioneering work illustrating that the complete conformal hydrolysis is the key to the improved supercapacitor performances of the MOF-derived Ni(OH)2 electrodes. The prepared Ni(OH)2 electrode under the optimized conditions has a specific capacity of 713.2 C g−1 at a current density of 1 A g−1, which is at least 28% larger than those of the Ni(OH)2 prepared at other temperatures. The detailed analyses based on CV and EIS of the obtained Ni(OH)2 electrodes indicate that the residual MOFs within electrodes due to incomplete hydrolysis significantly influence the diffusion length and diffusion efficiency of OH−, drastically lowering the supercapacitor performances.
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JOURNAL OF POWER SOURCES
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2019
·
IF 7.467
Yudi Niu,Xing Qian,Jiahao Zhuang,Hongyu Liu,Linxi Hou
Owing to the modifiable compositions and morphologies, high-efficiency clean energy catalysts with complex functional structures attract wide-ranging attention. Herein, this report focuses on the controllably morphological MoS 2 -doped NiS 2 /Co 3 S 4 nanocubes which are derived from nickel-cobalt Prussian-blue analogs. After annealing in N 2 flow, MoS 2 /Ni-CoS x porous nanocubes are prepared via regulating the reactant ratios (1/2, 1/1 and 2/1) between (NH 4 ) 2 MoS 4 and Ni–Co Prussian-blue analogs. In the synthesis progress, (NH 4 ) 2 MoS 4 is applied as a bifunctional dopant source, which can expediently offer Mo and S elements simultaneously. The quaternary porous MoS 2 /Ni-CoS x (1/1) with the reasonable chemical composition, considerable specific surface area (86.7 m 2 g −1 ) and excellent electrocatalytic property can be selected as the representative counter electrode catalyst in dye-sensitized solar cells. Furthermore, the solar cell with MoS 2 /Ni-CoS x (1/1) exhibits a higher power conversion efficiency (9.80%) than that of Pt (8.19%) under a standard irradiation.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2019
·
IF 4.978
Atian Xie,Jiuyun Cui,Yangyang Chen,Jihui Lang,Chunxiang Li,Yongsheng Yan,Jiangdong Dai
Realization of fast, efficient and continuous oil–water separation is of great significance for solving the problem of oil pollution. We present here a facile hydrothermal strategy to synthesize a superhydrophilic platanus fruit-like Ni@Ni(OH) 2 hierarchical architecture (SI-PFHA). Additionally, superhydrophobic platanus fruit-like Ni@Ni(OH) 2 hierarchical architecture (SO-PFHA) is obtained through stearic acid modification of SI-PFHA. Dual-channel separation system is integrated based on two superwetting membranes. Such separation system is competent for continuous light/heavy oil–water separation with high flux and high separation efficiency. Importantly, outstanding durability and reusability make this separation system a promising strategy for practical application in remediation of oily wastewater.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2014
·Vol. 39
·期 7
·3313-3319
·
IF 2.93
Jing Lin,Fei Liang,Yaoming Wu,Wanqiang Liu,Limin Wang
We prepared Ti 1.4 V 0.6 Ni ribbons by arc-melting and subsequent melt-spinning techniques. Ti 1.4 V 0.6 Ni + x Mg ( x = 1, 1.5, 2, 2.5 and 3, wt.%) composite alloys were obtained by the mechanical ball-milling method. The structures and hydrogen storage properties of alloys were investigated. Ti 1.4 V 0.6 Ni + x Mg composite alloys contained icosahedral quasicrystalline phase, Ti 2 Ni-type phase, β-Ti solid-solution phase and metallic Mg. The electrochemical and gaseous hydrogen storage properties of alloys were improved with Mg addition. Ti 1.4 V 0.6 Ni + 2 Mg alloy showed maximum electrochemical discharge capacity of 282.5 mAh g −1 as well as copacetic high-rate discharge ability of 82.3% at the discharge current density of 240 mA g −1 compared with that of 30 mA g −1 , and the cycling life achieved above 200 mAh g −1 after 50 consecutive cycles of charging and discharging. The hydrogen absorption/desorption properties of Ti 1.4 V 0.6 Ni + x Mg ( x = 1, 2 and 3, wt.%) alloys were better than Ti 1.4 V 0.6 Ni. Ti 1.4 V 0.6 Ni + 3 Mg alloy also exhibited a favorable hydrogen absorption capacity of 1.53 wt.%. The improvement in the hydrogen storage characteristics caused by adding Mg may be ascribed to better hydrogen diffusion and anti-corrosion ability.
研究领域:
材料科学
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金属功能材料
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储能材料
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物理化学
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电化学
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Zhengwen Li,Jiajun Zhang,Wei Pan,Shuairen Qian,Yuhan Wang,Dong Su,Liguo Wang,Binhang Yan
Single-atom catalysts for alkyne semi-hydrogenation have been extensively investigated due to their high metal utilization and improved olefin selectivity. However, their reactivity is hindered by the sluggish activation of reactants on isolated sites. Herein, a non-precise metal catalyst consisting of Ni-Cu hetero-diatomic pairs was prepared using a sequential deposition method. The diatomic sites catalyst exhibited an unprecedented activity among non-precious catalysts with over 98% conversion and 77 mol C2H2 mol metal −1 h −1 at 180 °C, whereas the single-atom catalysts of Cu/C and Ni/C were almost inert under the same conditions. Experimental and theoretical results revealed the crucial diatomic synergy between the Ni-Cu pairs, wherein acetylene was adsorbed on Ni sites and hydrogen was adsorbed on Cu sites, and the diatomic site enabled spontaneous desorption of ethylene. The superior activity of the diatomic catalyst was observed, resulting from the enhanced dominance of d -electrons of Ni near the Fermi level. The research demonstrates an approach to designing non-precise metal catalysts with extraordinary catalytic performance for alkyne hydrogenation.
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