ChemCatChem
·
2018
·Vol. 10
·期 20
·4689-4698
·
IF 4.674
Yan Liu,Ye Wu,Zarina Akhtamberdinova,Xiaoping Chen,Guodong Jiang,Dong Liu
Graphical High fives ! The catalyst 5Ni-5Ce exhibits the best catalytic performance in the dry reforming of shale gas and CO 2 . The introduction of Ce creates strong interaction between Ni and Ce, which enhances the electron transfer between them. And the substitution of Ni for Ce produces oxygen vacancies and defects, which can accelerate the adsorption and activation of the reactant gases molecule, further promoting the reaction. The dry reforming of shale gas (methane and ethane with an average ratio of 4 : 1) with carbon dioxide (DRS) is considered to be a promising way to produce syngas, which widens the utilization of shale gas and mitigates carbon dioxide emission. In this paper, Ce modified Ni-based catalysts were developed and the corresponding catalytic performances for DRS were investigated with a fixed bed reactor. Results showed that the catalyst containing 5 wt% of Ni and 5 wt% of Ce performed a best catalytic effect, including the selectivity of syngas and the carbon resistance performance, which is due to the good metal dispersion, strong interaction between Ni and Ce, and the formation of Ni-CeO x solid solution. The electron transfer between Ni and Ce, substitution of Ni for Ce, and the sequential oxygen vacancies or defects, play significant roles in activating CH 4 , C 2 H 6 and CO 2 . The conversion of reactant gas increased with temperature, while the selectivity of syngas is little affected with temperature. In addition, the desired catalyst containing 5 wt% of Ni and 5 wt% of Ce showed good stability in the long-time operation, which indicates that the Ce modified Ni-based catalyst is a promising one for the dry reforming of shale gas.
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RSC Advances
·
2024
·Vol. 14
·期 52
·39061-39068
·
IF 3.9
Han Xiao,Jiaming Dong,Yimin Zhang,Xiaohua Cao,Yanhong Li,Dedong He,Yongming Luo,Pingyan Wang,Hao Wang
The presence of abundant hydroxyl groups on the surface of Al2O3 can promote the dispersion of Ni species but produce an inactive NiAl2O4 phase at high temperatures. Moreover, the catalysts prepared by the conventional incipient wetness impregnation method lack the sites for the activation of CO2, which leads to coke deposition and thus affects the catalyst activity. The above restricts the utilization of Ni in conventional Ni/Al2O3 catalysts. In this paper, Al2O3 support was pre-treated by acetic acid to selectively remove hydroxyl groups without affecting the coordination environment of Al. Results revealed that the Al2O3 support after hydroxyl removal not only showed moderate metal–support interaction but also produced more sites for the adsorption and activation of the reactant, which significantly improves the utilization of nickel species and the stability of the catalyst. The conversion of CH4 and CO2 at 700 °C was as high as 88% and 90%, respectively, and has an excellent stability of 50 h. This study provides a feasible strategy for the design of highly active methane dry-reforming catalysts.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuzhu Xue,Weinan Wang,Yanhong Zhang,Qinhua Fan,Ying Zhang,Chen Ling,Yuwei Pan
This study proposes a green purification strategy in which mild decomplexation of Ni-EDTA into other Ni complexes facilitates the efficient removal and recovery of nickel through resin adsorption. Decomplexation of Ni-EDTA by boron/Fe 2+ /H 2 O 2 (B/Fe 2+ /H 2 O 2 ) followed by resins adsorption was conducted for Ni(II) removal in Ni-EDTA. The Ni(II) removal efficiency could only achieve 1.3 % and 6.2 % while Ni(II) coexisted with EDTA but more than 10 times of higher when Ni(II) coexisted with EDTA-relatives via the single adsorption of commercial heavy metal-affined resins (D001 and D463), which attributed to the increased binding energies of these Ni-EDTA’s degradation products complexes than Ni-EDTA based on density functional theory (DFT) calculation. In comparing to precipitation, the resin adsorption required much less mineralization of EDTA to have a better removal efficiency of Ni(II). B improved the efficiency of Ni-EDTA decompexation by accelerating the recycle of Fe 3+ /Fe 2+ . The EDTA (and TOC) removal enhanced from 48.7 % (4.7 %) to 94.7 % (11.9 %) by B/Fe 2+ /H 2 O 2 process comparing to Fe 2+ /H 2 O 2 process. With the high EDTA but low TOC removal efficiency after B/Fe 2+ /H 2 O 2 treatment, Ni(II) removal efficiency via resins adsorption could maximum achieve 80.5 %, 2–3 times of that via regular precipitation method. In addition, B and resins exhibited good reusability in five cycles, and B/Fe 2+ /H 2 O 2 -resins process had excellent adaptability to different heavy metal complexes. B/Fe 2+ /H 2 O 2 -D463 system not only could reduce 78.4 % reagents cost compared with that of Fe 2+ /H 2 O 2 -precipitation process, but also could save much cost than other processes. The results provide new insights for the cost-effective treatment of EDTA-complexed heavy metal wastewater.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Liang Ding,Roujia Zhang,Peng Zhao,Changsheng Qu
Based on the remediation challenges and practical needs of trichloroethylene (TCE)-contaminated groundwater, this study prepared an Ni-based composite electrode, Pd/Ni(OH) 2 /Ni foam (NF), and evaluates its electrocatalytic degradation effect on TCE in a groundwater environment. Under an applied voltage of –1.3 V versus Ag/AgCl, the TCE removal rate reaches 95% after 3 h of electrolysis. The introduction of Ni(OH) 2 nanoarrays accelerates the electron transport process, shortens the ion transport distance, and significantly increases the electron density of Pd. Furthermore, TCE is rapidly reduced by adsorbed hydrogen radicals on the Pd surface, and the ethane conversion rate reaches 62%. The experimental results show that the electrode can maintain a strong electrocatalytic activity over a wide pH range (3–9) and that it is not affected by common anions, such as Ca 2+ , HCO 3 - , SO 3 2- , or Cl - , in groundwater. Pd/Ni(OH) 2 /NF exhibits a high reactivity after six cycles of use. The remediation mechanism is studied by combining the microscopic characterization of materials, electrochemical activity testing, and process product identification, which provides an effective way of completely degrading chlorinated hydrocarbon pollutants in natural groundwater environment.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Yue Liu,Wei Peng,Hancheng Ma,Jinsai Tian,Kao Wang,Zhaobo Zheng,Lin Xu,Yao Ding
Metal–organic frameworks have aroused growing interest in the research of energy conversion and storage. However, their specific configuration, especially the coordination environment of metal active sites, has not been well designed. Their role in regulating the structural reconstruction of pre-electrocatalysts remains ambiguous. Herein, this work reports a dual-ligand strategy to design a Ni-MOF with asymmetric Ni–O coordination, named Ni–BDC–DOBDC, which occupies unsaturated Ni sites and strengthens Ni–O bonds. As inspected by X-ray absorption near edge structure as well as a series of in situ and ex situ characterizations, this special Ni–O coordination contributes to Ov-NiOOH with rich oxygen vacancies during fast self-reconstruction at a lower potential. Moreover, theoretical results reveal that Ni sites in Ov-NiOOH occupy a higher d-band center, a lower adsorption energy barrier, and a more electronic negative surface in the oxygen evolution reaction, leading to good electrocatalytic performance. Overall, Ni–BDC–DOBDC catalysts exhibit a low overpotential of 202 mV at 10 mA cm–2 and outstanding stability within 240 h. The insights in this work pave the way for high-performance MOF-based catalysts by regulating their self-reconstruction kinetics through a new aspect of asymmetric ligand engineering.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Chen Ling,Zixi Ren,Mengmeng Wei,Fei Tong,Yuwei Cheng,Xiaopeng Zhang,Fuqiang Liu
Inorganic complexants, such as ammonia (AA) and pyrophosphate (PP), are often present alongside heavy metal ions in alkaline plating rinsing wastewater. We investigated the removal capacity of Ni(II) from waters containing [Ni-xNH 3 -yP 2 O 7 ] n complexes by chelating and ion-exchange resins in sole and dual-ligand systems. D463 (containing iminodiacetic groups) and PAMD (possessing polyamine groups) exerted superior performance under all conditions. Ni(II) adsorption on D463 decreased with AA and PP by 10.3% and 64.4%, respectively. Conversely, the adsorption on PAMD increased by 57.3% and 75.8%, respectively. PAMD exhibited high selectivity toward anionic [Ni-PP] species over free PP. More Ni(II) was captured by PAMD in the dual-ligand systems than sole systems, while the case for D463 was opposite. As confirmed by species tracking and DFT/XPS analyses, complexes breaking-Ni 2+ capture was the dominant mechanism for D463, while the dual-site (non-charged and protonated amines) interactions with NiP 2 O 7 2– on PAMD promoted its adsorption. The tandem combination D463-PAMD was the optimal mode to remove the most Ni(II). The actual wastewater test demonstrated that >210 BV effluent met the limit of 0.1 mg Ni(II)/L and the eluent contained 15 g Ni(II)/L. This study guides the application of chelating adsorption processes in the advanced treatment of plating rinsing wastewaters.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Mingdong Sun,Shibo Xi,Siyu Zhu,Yu Zhou,Changping Li,Biao Meng,Jiao Wei,Xiao Chi,Xiaojiang Yu,Yujie Cao,Yizhong Huang,Xiaoling Liu,Jun Wang
N-doped carbon-supported single-atom metal sites (Me−N−C) have emerged as promising candidates for electrochemical CO 2 reduction reaction (CO 2 RR) under industrial current densities. However, rationalizing their local coordination environment remains challenging. Herein, a feasible strategy is demonstrated for constructing robust Ni─N─C centers by designing a new family of single-crystalline ionic ZIF-8 materials with atomically defined ionic liquid (IL) cations inside the microchannels. The ─COOH tethered ionic ZIF-8 directed the formation of atomically dispersed Ni─N 4 sites with an elongated Ni─N bond of 1.94 Å. The resulting Ni─N─C catalyst effectively catalyzed the electrochemical CO 2 reduction to CO, delivering a partial current density of 679 mA cm −2 with a Faradic efficiency of 97% and achieving a maximum turnover frequency of 106197 h −1 . The extended Ni─N bond enables the slightly reduced valence state of the Ni site, optimizing the affinity toward CO 2 and intermediate, and thus lowering the energy barrier in the rate-determining * CO 2 → * COOH step.
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Molecular Catalysis
·
2021
·
IF 5.062
Zhige Zhang,Guofeng Zhao,Bing Han,Jiawei Zhong,Jun Xie
Sustainable transformation of methane into methanol feedstock syngas is a promising direction in future energy generation. A monolithic SiC-foam (SiC-foam, denoted as SCf) supported structured Ni-SrO composite nanomaterial was prepared via reducing the SrNiO 3 perovskite. The Ni-SrO/SCf displays a stronger resistance to Ni-sintering/coke-deposition than the unmodified Ni/SCf due to its uniform Ni distribution as well as the strong Ni-SrO interaction. In the presence of Ni-SrO/SCf sample at a gas hourly space velocity (GHSV) of 24,000 mL CH4 CO2 g Cat −1 h − 1 and an operating temperature of 850 °C, the initial conversion rate of biogas (CH 4 /CO 2 ) was 70/94%, which gradually dropped to 55/72% within 40 h, but its activity remained stable for the next 60 h. By contrast, the conversion rate of biogas (CH 4 /CO 2 ) in the presence of Ni/SCf sample was decreased rapidly from 60/80 to 50/65% within 20 h, due to the severe coke deposition and Ni-sintering.
研究领域:
能源化学
·
催化材料科学
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Nanoscale
·
2022
·Vol. 14
·期 39
·14779-14788
·
IF 8.307
Changle Fu,Liangliang Feng,Hongyan Yin,Yuhang Li,Yajie Xie,Yongqiang Feng,Yajuan Zhao,Liyun Cao,Jianfeng Huang,Yipu Liu
Developing low-cost, environmentally friendly and efficient non-precious metal electrocatalysts as alternatives to noble metals for the hydrogen evolution reaction (HER) is highly essential for the sustainable advancement of green hydrogen energy. Herein, a novel heterostructured Ni3P/Ni nanoparticle anchored in nitrogen-doped mesoporous carbon nanofibers (Ni3P/Ni@N-CNFs) is prepared by a facile solid-phase calcination protocol. The results demonstrated that benefiting from the intensive electronic coupling effect at the interface of the Ni3P/Ni heterostructure, the electron configuration of the Ni active site is optimized and thus the favorable HER activity. Furthermore, the N-doped carbon nanofiber scaffold with an extensive mesoporous structure endows Ni3P/Ni@N-CNFs with abundant electrochemically active sites together with excellent conductivity and stability, contributing to fast electron/mass transport. As expected, the resultant Ni3P/Ni@N-CNF electrocatalyst exhibited exceptional HER catalytic properties under universal pH conditions, driving a current density of 10 mA cm−2 at pretty low overpotentials of 121 mV, 145 mV and 187 mV in acidic, basic and neutral solutions, respectively, and retaining the catalytic stability for over 60 h. This intriguing work represents a fresh perspective for designing and exploiting highly advanced phosphide electrocatalysts for green hydrogen fuel production.
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Lin-Chang Liu,Hong-Lin Zhu,Yue-Qing Zheng
Ammonia borane (NH3BH3, referred to as AB) hydrolytic dehydrogenation is regarded as a feasible strategy for hydrogen production owing to its high hydrogen content, pollution-free nature, and high stability. Metal nitrogen-doped carbon materials (M-N-C) are considered as an ideal candidate support of catalysts with AB hydrolytic dehydrogenation due to the advantages of low cost, large specific surface area, rich defective site, and good chemical stability. In this work, tubular Ni@Ni-N-C was successfully synthesized by high-temperature pyrolysis, and then, Rh nanoparticles were decorated on the support Ni@Ni-N-C by impregnation and reduction to prepare a series of Rh/Ni@Ni-N-C. The best catalytic performance of catalysts is obtained using Ni@Ni-N-C with an Rh loading of 0.74 wt %, showing a turnover frequency as high as 782.18 min–1 and an apparent activation energy (Ea) as low as 25.86 kJ mol–1, which could be attributed to the strong interaction between Rh and the defective site of the support.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Fuhuan Wang,Yucan Liu,Jiakun Sun,Hewu Wang,Dongsheng Ren,Languang Lu,Pengfei Yan,Youpeng Chen,Haoran Hu,Minggao Ouyang
Solid oxide fuel cells (SOFCs) have gained significant attention as highly efficient energy conversion devices. Enhancing the overall performance of SOFCs relies on the development of efficient anode materials. In this study, an impregnation approach is proposed to improve the electrochemical performance of the nanocomposite Ni-GDC anode by modulating oxygen vacancies and Ni dispersion. This method successfully achieves well-dispersed Ni nanoparticles and adequate oxygen vacancies in the NiO-GDC anode, resulting in excellent TPBs and catalytic activity for SOFCs. The NiO-GDC nanocomposite exhibits a significant improvement in electrochemical activity, reaching a peak power density of 0.37 W/cm2 at 850 °C. Moreover, it demonstrates remarkable durability with a degradation rate of only 0.1%/h at −380 mA/cm2. This study provides valuable insights into the modulation of oxygen vacancies and Ni dispersion in nanocomposite Ni-GDC anodes, underscoring their potential as high-performance materials for solid oxide fuel cells. These findings contribute to the advancement of superior anode materials with improved electrochemical performance, holding tremendous potential for the development of more efficient and reliable SOFCs.
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NANOTECHNOLOGY
·
2021
·Vol. 32
·期 34
·345706
·
IF 3.874
Leqiu He,Yan Wang,Yajie Guo,Guobing Li,Xubin Zhang,Wangfeng Cai
Novel core−shell nanostructure electrodes benefit from the excellent properties of their constituent materials, as well as the synergy between them. However, it is challenging to fabricate such structures efficiently. In this study, NiSe nanorods were fabricated using Ni foam as the conductive substrate and reactant via a one-step hydrothermal process, and Ni(OH)2 nanosheets were coated on the surface of the nanorods via one-step electrodeposition. The effect of the structure and morphology on the properties of the material was explored using scanning electron microscopy, x-ray diffraction, and electrochemical technology. The obtained core−shell NiSe/Ni(OH)2 exhibited an areal capacity of 1.89 mAh cm−2 at a current density of 5 mA cm−2. The assembled NiSe/Ni(OH)2//AC hybrid supercapacitor exhibited excellent energy and power densities, indicating that NiSe/Ni(OH)2 has great potential for use as a battery-type electrode in energy storage systems.
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