CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Huan Lv,Shengyan Meng,Zhaolun Cui,Shangkun Li,Dongxing Li,Xiaoxia Gao,Hongchen Guo,Annemie Bogaerts,Yanhui Yi
Efficient methane conversion to methanol remains a significant challenge in chemical industry. This study investigates the direct oxidation of methane to methanol under mild conditions, employing a synergy of non-thermal plasma and Cu-MOR (Copper-Mordenite) catalysts. Catalytic tests demonstrate that the Cu-MOR IE-3 catalyst (i.e., prepared by three cycles of ion exchange) exhibits superior catalytic performance (with 51 % methanol selectivity and 7.9 % methane conversion). Conversely, the Cu-MOR catalysts prepared via wetness impregnation tend to over-oxidize CH 4 to CO and CO 2 . Through systematic catalyst characterizations (XRD, TPR, UV–Vis, HRTEM, XPS), we elucidate that ion exchange mainly leads to the formation of zeolite-confined Cu 2+ species, while wetness impregnation predominantly results in CuO particles. Based on the catalytic performance, catalyst characterizations and in-situ FTIR spectra, we conclude that zeolite-confined Cu 2+ species serve as the active sites for plasma-catalytic direct oxidation of methane to methanol.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Shuli Yin,Songliang Liu,Ziqiang Wang,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Thermodynamically favorable oxidation reaction instead of oxygen evolution reaction (OER) with sluggish kinetics as anode reaction and coupled with hydrogen evolution reaction (HER) at cathode is an effective hydrogen production technology . Herein, we report a solvothermal method synthesis of defect-rich crimped perforated PdIn bimetallene as an efficient catalyst for hydrogen production with the assistance of methanol. Boosted by abundant crystal defects , higher surface energy and expanded surface active sites, the defect-rich crimped perforated PdIn bimetallene exhibits superior activity and stability in catalyzing methanol oxidation reaction (MOR) and HER. At the established MOR-HER co-electrolytic system, when the anode and cathode are equipped with PdIn bimetallene, the required cell voltage only is 1.26 V to achieve the current density of 100 mA cm −2 , which is 0.93 V lower than that of traditional water electrolysis. This work reports a defect-rich crimped perforated PdIn bimetallene catalyst, as an effective bifunctional catalyst that provides insight for the advancement of energy-saving and promising hydrogen production engineering.
研究领域:
催化
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氢能
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材料科学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Kaiyu Dong,Houkang Pu,Te Zhang,Huizhen Dai,Xihui Zhao,Luming Zhou,Kuankuan Wang,Yingying Wang,Yujia Deng
Designing and modulating the morphological structure of catalysts is of great significance to improve their catalytic activity and stability. In this work, PtRu alloy nanodendrites with tunable components were constructed by the introduction of Ru. Owing to the presence of electron transfer in the alloy nanocatalysts and their unique nanodendritic structures, Pt 0.8 Ru 0.2 alloy nanocatalysts with optimal composition exhibited excellent electrocatalytic activity and stability in ethylene glycol oxidation reaction (EGOR) and methanol oxidation reaction (MOR). Among the nano-catalysts, mass activities of Pt 0.8 Ru 0.2 nanodendritic catalysts to EGOR and MOR were 6.1 A mg −1 and 4.6 A mg −1 , and the specific activities were 11.5 mA cm −2 and 8.68 mA cm −2 , respectively, much better than those of commercial Pt/C catalysts. This work provides a strategy for designing efficient PtRu catalysts for fuel cells.
研究领域:
催化
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纳米材料
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电化学
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燃料电池
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产品关联
DOI
高影响因子
ChemCatChem
·
2023
·Vol. 15
·期 15
·e202300300
·
IF 4.5
Yanxin Bai,Hui Xiong,Zhao Jiang,Riguang Zhang,Tao Fang.
Graphical The TNNs-modified Ni/C catalysts (TM=V, Mo, Nb, Ta) exhibited higher activity, kinetics, charge transfer and stability for alkaline MOR. Ni/VN−C showed the highest catalytic activity, nearly three times higher than that of Ni/C due to the highest coverage of the surface component NiOOH. A volcano plot existed between the d-band center and activity of the corresponding catalysts. Transition metal nitrides are considered as the promising materials in the energy conversion processes due to the similar electronic structures to Pt. In this work, a series of Ni/TMN−C (TM=V, Mo, Nb, Ta) catalysts were synthesized and investigated the catalytic performance for methanol oxidation reaction in alkaline media. The electrochemical measurements indicated that the TNNs-modified Ni/C catalysts exhibited higher activity, kinetics, charge transfer and stability for alkaline MOR compared with Ni/C. It was found that the incorporation of TMNs improved the activity and stability for MOR in various degree. Specially, Ni/VN−C showed the highest catalytic activity, nearly three times higher than that of Ni/C due to the highest coverage of the surface component NiOOH, consistent with the Tafel and EIS results that it exhibited the fastest charge transfer kinetics and reaction rate. XPS characterization indicated that the obvious electron interaction occurred between the TMNs and Ni species and Ni would transfer electrons to the transition metal nitrides, resulting in the electron-rich states of TMNs. Interestingly, combining the d-band center and activity of the corresponding catalysts, it could be found that a volcano plot existed between them, suggesting that the introduction of appropriate nitrides would change the electronic structure of Ni and enhance the catalytic performance for MOR in alkaline media.
研究领域:
材料科学
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电化学
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催化科学
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产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
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2025
·
IF 5.6
Hui Xiong,Xinyi Hu,Xiaoying Qi,Zhao Jiang
It is essential to design and produce stable, high-activity, and low-cost anode catalysts for direct methanol fuel cells (DMFCs). To improve the efficiency of the methanol oxidation reaction (MOR) in alkaline media, a series of PdM-NbN/C (M=Co, Ni, Cu) bi-component catalysts were synthesized by introducing various oxyphilic metals. Electrochemical evaluations show that the presence of Ni and Co significantly enhances catalytic activity, charge transfer kinetics, CO tolerance, and long-term stability compared to Pd-NbN/C. Among these, PdNi-NbN/C exhibits the highest mass activity of 4806.67 A·g Pd −1 , the lowest onset potential and charge transfer resistance, as determined from electrochemical testing. The rate-determining step (RDS) is identified as the CO ads oxidation reaction. Characterization analysis confirms that the second oxyphilic metals primarily optimize the Pd electronic structure and modulate the interaction between Pd and NbN, making a favorable shift in the d-band centers. Additionally, Ni and Co elements tend to form hydroxides in higher proportions, which aids in the removal of CO ads and accelerates the RDS. The electronic interactions between Pd, Ni, and NbN species are key to the enhanced catalytic performance for MOR. Pd nanoparticles in the electron-deficient condition may aid in the activation of methanol and its intermediates, as indicated by the linear relationship between the mass activities and d-band centers. This work offers important information for the logical design of efficient anode catalysts for DMFCs.
研究领域:
材料科学
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电化学
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燃料电池
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2020
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IF 2.627
Shenglai Li,Lisong Fan,Lina Song,Dangguo Cheng,Fengqiu Chen
Iron-containing zeolites play an important role in the selective oxidation of methane to oxygenates by nitrous oxide. A solid-state ion exchange method is adopted to prepare Fe-MOR zeolite catalysts with different amounts of extra-framework Al. EPR spectra and UV–vis spectra show that the percentage of iron ions in tetrahedral or octahedral coordination increases while those of clustered Fe species decrease by the addition of extra-framework Al species. Nitrous oxide titration reveals that more active Fe centers are formed, which promote the nitrous oxide consumption. The number of active centers in the catalyst with the introduction of extra-framework Al is about four times that of the catalyst without the addition of extra-framework Al. Due to this, there is an increase in the methane conversion, total selectivity and yield of oxygenates.
研究领域:
化学
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催化作用
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Xiaolan Li,Yangqi Huang,Zhenyu Chen,Shuqi Hu,Jinliang Zhu,Panagiotis Tsiakaras,Pei Kang Shen
A series of tri-functional nanoflower (NF) catalysts with numerous nanodendrites (Pt 3 NiRh, Pt 3 NiRu, Pt 3 NiPd, Pt 3 Ni, and Pt 2 Ni 2 Rh NFs) were synthesized by introducing Rh, Ru, and Pd into Pt-Ni nanoflowers, aiming at accelerating the sluggish kinetics of oxygen reduction reaction (ORR), methanol oxidation reaction (MOR), and hydrogen evolution reaction (HER). The as-prepared catalysts displayed superior anti-poisoning ability and excellent activity due to uniform morphology and good dispersibility. Their electrochemical characterization revealed that the Pt 3 NiRh NFs showed the highest mass activity (2.17 A m g P G M - 1 ) and specific activity (3.13 mA cm -2 ) toward ORR, close to 9.9 and 4.6 times higher than the values measured on Pt/C (46.7 %). As for MOR, mass and specific activities of Pt 3 NiRh NFs were 1.88 A m g P G M - 1 and 2.62 mA cm -2 , far exceeding the values on commercial Pt/C. Moreover, HER activity of Pt 3 NiRh NFs outperformed commercial Pt/C. This work is valuable to develop promising multi-functional catalysts with enhanced activity and anti-poisoning ability.
研究领域:
材料科学
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电化学
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催化领域
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产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2017
·Vol. 164
·期 4
·B92
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IF 3.259
Jingchao Zhang,Chunying Xu,Daojun Zhang,Jingli Zhao,Shuxian Zheng,Huimin Su,Feifei Wei,Baiqing Yuan,Carlos Fernandez
The synthesis of a novel hierarchical flower-like NiS via a solvothermal method for the electrochemcial oxidation of H2O2 on a carbon paste electrode with high catalytic activity for the (MOR) in an alkaline medium has been reported. Novel nickel sulfide (NiS) hierarchical flower-like structures were characterized by X-ray diffraction, scanning electron microscope, and transmission electron microscopy. A carbon paste electrode was modified with the as-prepared hierarchical flower-like NiS, resulting in a high electrocatalytic activity toward the oxidation of H2O2. The NiS-modified electrode was used for H2O2 sensing, which was achieved over a wide linear range from 0.5 μM to 1.37 mM (I/μA = −0.19025 + 0.06094 C/mM) with a low limit of detection (LOD) of 0.3 μM and a limit of quantitation (LOQ) of 0.8 μM. The hierarchical flower-like NiS also exhibited a high electrocatalytic activity for the methanol oxidation reaction (MOR) in an alkaline medium with a high tolerance toward the catalyst-poisoning species generated during the MOR. The MOR proceeded via the direct electrooxidation of methanol on the oxidized NiS surface layer because the oxidation peak potential of the MOR was more positive than that of the oxidation of NiS.
研究领域:
材料科学
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电化学
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分析化学
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DOI
高影响因子
Advanced Sustainable Systems
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2025
·
IF 6.1
Haiyu Ma,Jian Li,René Hübner,Xingyu Tao,Kairui Xu,Mingjia Lu,Jiakun Du,Muwu Li,Zhikun Zheng,Wei Liu
Platinum-based electrocatalysts represent the most promising candidates for the methanol oxidation reaction (MOR) in direct methanol fuel cells. However, the wide commercialization of platinum-based electrocatalysts faces significant challenges, including high material costs, insufficient catalytic activity, limited operational durability, and susceptibility to CO poisoning. To overcome these issues, a new Au-doped Pt-Co aerogel (AG) is fabricated by the facile one-pot aqueous-solution heteroatom doping method. This catalyst demonstrates good electrocatalytic performance for MOR, combining both high activity and remarkable stability. The Au 1 -Pt 67 Co 33 AG with optimized Au doping amount exhibits outstanding mass activity, which is 1.7 times that of its undoped Pt 67 Co 33 AG counterpart and 4.6 times that of the commercial Pt/C catalyst. Furthermore, the Au 1 -Pt 67 Co 33 AG demonstrates significantly enhanced long-term stability under continuous operation. Density functional theory calculations indicate that Au doping reduces the energy barriers for methanol dehydrogenation and lowers the total energy barriers for the *CO oxidation steps, facilitating the rapid dehydrogenation of CH n OH and faster conversion of *CO, thereby significantly enhancing the electrocatalytic activity and stability of the Au 1 -Pt 67 Co 33 AG toward MOR.
研究领域:
电化学
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催化
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材料科学
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纳米技术
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能量转换
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Feng Yu,Yuqin Li,Dengke Cheng,Bowen Chen,Wuwen Si,Yan Wang,Yonghao Li,Xiaowei Wu,Tian Gui,Xiangshu Chen,Hidetoshi Kita
Abstract The rapid preparation of high-performance MOR zeolite membranes for the dehydration of high-concentration acetic acid under fluoride-free conditions remains a significant challenge. In this study, a hydroxyl radical-promoted strategy was successfully applied to fabricate high-performance MOR zeolite membranes on macroporous mullite supports within only 3 h, under fluoride-free and organic-template-free conditions. The formation process of MOR zeolite membranes in the presence of hydroxyl radicals was systematically investigated. Furthermore, the roles of hydroxyl radicals and hydroxide ions in the synthesis mechanism of MOR zeolite membranes were discussed in detail using characterization methods such as SEM, XRD, EPR, and fluorescence spectroscopy. Compared with the synthesis system without hydroxyl radical participation, the hydroxyl radical-promoted MOR zeolite membranes not only exhibited a significantly shortened crystallization time but also enabled a reduction in the alkalinity of the reaction system. The membrane prepared under optimal conditions demonstrated excellent separation performance in a 90 wt % acetic acid/water mixture at 75 °C, with a permeation flux as high as 1.37 kg m–2 h–1 and a water content in the permeate exceeding 99.4 wt %. Moreover, the MOR zeolite membranes prepared using the hydroxyl radical-promoted strategy showed excellent reproducibility. This hydroxyl radical-promoted approach provides an efficient and environmentally friendly route for the rapid preparation of high-performance zeolite membranes under fluoride-free, template-free, and low-alkalinity conditions.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Feiyan Si,Shuai Wang,Yanao Zhang,Ruixin Xue,Yipin Lv,Guozhu Chen,Daowei Gao
Addressing the pivotal challenge of lattice distortion and electronic structure modulation in High-Entropy Alloys (HEAs) for electrochemical catalysis, this investigation presents the synthesis of a novel PtRhNiCoFeGaW HEA in a three-dimensional nanoflower configuration. This design strategically combines enhanced morphological features and a synergistic metallic interaction, propelling the catalytic efficiency forward in methanol and formic acid oxidation reactions (MOR and FAOR). The synthesized HEA nanoflowers exhibit superior mass and specific activities of up to 1.34 mA μg Pt −1 and 4.43 mA cm −2 for MOR, alongside 0.52 mA μg Pt −1 and 1.74 mA cm −2 for FAOR , markedly surpassing those of conventional Pt/C and PtRhNi NFs. This leap in performance is primarily attributed to the intricate elemental synergy within the HEAs, which effectively minimizes CO poisoning (a notorious catalyst deactivator) by improving CO* resistance. Furthermore, the study delineates how the unique nanoflower morphology contributes to exposing a plethora of active sites, thereby maximizing catalytic action. This research not only navigates through the complexities of crafting multi-elemental catalytic systems but also establishes a foundational strategy for developing next-generation HEA-based electrocatalysts, poised to significantly impact future advancements in energy conversion technologies.
研究领域:
材料科学
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电化学
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催化
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纳米技术
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2019
·
IF 0
Ting Qu,Qiang Tan,Yingjie Chen,Liting Liu,Shengwu Guo,Yuanzhen Chen,Yan Liu,Sai Li,Yongning Liu
Direct alcohol fuel cell technology (DAFC) has gained significant interest recently as it is a green energy technology with a low/zero pollution emission. Nevertheless, the sluggish kinetics of the electrocatalysis process and the high cost of anode catalysts still impede the wide application of DAFC. Moreover, the limited understanding of the reaction mechanism restrains the development of anode catalysts. Here, we have prepared a Pd-(SnO2@C)/C catalyst and highlighted a strategy to demonstrate the effects of active oxygen-contained species and electronic interaction, which are identified to have a synergistic effect. The as-prepared Pd-(SnO2@C)/C catalyst showed remarkable activity and stability for EOR and MOR in alkaline media. It also had an encouraging performance in a polymer fiber membrane-based alkaline DAFC, where a NiCo2O4 catalyst was used for the oxygen cathode. Combined with the theoretical analysis and the experimental research results, this study reveals that the electronic interaction is the dominant mechanism in the synergistic effect, which provides theoretical guidance and technical support for the preparation of the next generation of high catalytic activity and high stability anode catalysts of DAFC.
研究领域:
电化学
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催化
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能源材料
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燃料电池
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产品关联
DOI
危险品化学品经营许可证（带存储）