ACS Catalysis
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2020
·
IF 12.35
Hai-Bin Wang,Jia-Qi Wang,Rui Zhang,Chuan-Qi Cheng,Kang-Wen Qiu,Yi-jie Yang,Jing Mao,Hui Liu,Miao Du,Cun-Ku Dong,Xi-Wen Du
Highly effective catalysts are of great importance for artificial nitrogen fixation. Inspired by the natural nitrogenase, we biomimetically designed an inorganic catalyst, Mo(IV)-doped FeS2, for electroreduction of dinitrogen to ammonia. The Mo(IV) ions favor the adsorption and activation of N2, while the FeS2 substrate depresses the competitive hydrogen evolution reaction, and the two factors jointly endow the catalyst with a high Faraday efficiency of 14.41% at −0.2 V versus RHE.
研究领域:
生物化学
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材料科学
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产品关联
DOI
高影响因子
MOLECULES
·
2022
·Vol. 27
·期 21
·7617
·
IF 4.927
Xiaodong Fang,Xiangguo Wang,Ling Ouyang,Longcheng Zhang,Shengjun Sun,Yimei Liang,Yongsong Luo,Dongdong Zheng,Tairan Kang,Qian Liu,Feng Huo,Xuping Sun
The development of efficient electrochemical seawater splitting catalysts for large-scale hydrogen production is of great importance. In this work, we report an amorphous Co-Mo-B film on Ni foam (Co-Mo-B/NF) via a facile one-step electrodeposition process. Such amorphous Co-Mo-B/NF possesses superior activity with a small overpotential of 199 mV at 100 mA cm−2for a hydrogen evolution reaction in alkaline seawater. Notably, Co-Mo-B/NF also maintains excellent stability for at least 24 h under alkaline seawater electrolysis.Keywords:amorphous Co-Mo-B film;alkaline seawater electrolysis;hydrogen evolution reaction
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Xuan Liu,Chang’an Wang,Tao Zhu,Qiang Lv,Defu Che
In this paper, the simultaneous removal of SO 2 and NO x catalyzed by Fe-Mo mixed oxides at varying Mo/Fe atomic ratios was reported for the first time with the aim of reducing H 2 O 2 consumption and elucidating the roles of Fe and Mo species in the catalytic process. Fe-Mo mixed oxides with varying Mo/Fe atomic ratios were synthesized and the catalytic performances were systematically studied. The catalyst with Mo/Fe atomic ratio of 2.0 exhibited the highest activity, with which removal efficiencies of 89.4 % for NO x and 100 % for SO 2 can be attained at extremely low H 2 O 2 dosage. Products analysis revealed that SO 2 was mainly removed via wet scrubber, while the adequate oxidation resulting from OH radicals was the prerequisite for NO x removal. The redox pair of Fe 2+ /Fe 3+ played a significant role in decomposing H 2 O 2 , while Mo species had double effect on catalytic activity. Higher Mo content resulted in abundant oxygen vacancies and stronger surface acidity, which favored OH formation. However, the excessive Mo content involved severe surface Mo enrichment and remarkably reduced the active sites of Fe species. The H 2 O 2 /Fe-Mo catalyst system showed excellent stability and had a promising prospect for simultaneously removing SO 2 and NO x in coal-fired flue gas.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
INORGANIC CHEMISTRY
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2025
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IF 4.7
Qing-Shuai Zhang,Yu-Le Wang,Li Yue,Yu-Dong Shan,Song-Hai Wu,Yong Liu,Xu Han
Although selective oxidation of benzene to phenol (SOBP) by H2O2 is an important chemical process, overoxidation of benzene by the produced nonselective •OH during the activation of H2O2 inevitably reduces the oxidation selectivity. We, therefore, attempt to mediate the oxidation selectively by using electrophilic KHCO3 in the oxidation system. In this study, Mo–Cu/NC has been successfully synthesized via ball-milling bimetallic Mo–Cu and N-doped carbon, which exhibits high reactivity in SOBP by H2O2 and KHCO3 with a desirable phenol yield of 25.1% and selectivity of 100%. A series of characterizations and DFT calculations reveal that the reaction between H2O2 and KHCO3 produces HCO4–, which is then moderately activated on Mo1Cu2/NC via the nonradical pathway with the formation of Mo-(η2-O2) peroxo. Meanwhile, Ov at Mo1Cu2/NC facilitates the adsorption of benzene, which is then selectively oxidized by Mo-(η2-O2) peroxo to phenol via the oxygen atom transfer pathway. This study provides new insights on the importance of Mo-(η2-O2) peroxo mediated by H2O2–KHCO3 in selective oxidation of aromatic C–H bond via the nonradical pathway.
研究领域:
化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yanxu Wang,Lijia Huang,Tian C. Zhang,Yan Wang,Shaojun Yuan
Ammonia gas (NH 3 ) is a notorious malodorous pollutant with detrimental effects on environment and human health. Removing NH 3 through photocatalytic oxidation remains a challenging task due to unclear reaction mechanisms. In this study, DFT simulation results revealed that C doped TiO 2 could extend the photo-response range to the visible region, but the introduction of deep impurity levels was found to accelerate photogenerated carrier recombination. Fortunately, the rational doping of Mo was found to mitigate this negative effect. Accordingly, Mo, C co-doped TiO 2 was synthesized via a facile low-temperature calcination process, resulting in unique band structure that enhanced the photocatalytic oxidation of NH 3 . Notably, in-situ DRIFTS and DFT results demonstrated that the gradual reaction of NH 3 adsorbed on Mo atoms with oxygen species through the N 2 H 4 mechanism, promoting the formation of N 2 . These findings offer insights into the design of efficient photocatalysts for NH 3 removal under visible light, and present a promising technology for indoor air pollution control.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
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IF 6.76
Jiaqi Zhang,Quanhui Hou,Yanbing Liu,Xinglin Yang
The design of catalysts with excellent catalytic activity plays an important role in the field of solid-state hydrogen storage of new energy sources. Herein, a novel hydrangea-like NiO@NiMoO 4 composite catalyst was prepared through a facile hydrothermal reaction. Subsequently, NiO@NiMoO 4 was doped into MgH 2 by ball milling to solve the problems of high dehydrogenation temperature and slow desorption kinetics of MgH 2 . It can be seen from the experimental results that the MgH 2 + 10 wt% NiO@NiMoO 4 composite starts to dehydrogenate at about 190 °C, which is about 170 °C lower than that of pure MgH 2 . Meanwhile, after complete dehydrogenation, the composites can start to absorb hydrogen below 40 °C. Compared with pure MgH 2 , the activation energy of hydrogen absorption and dehydrogenation of the composite decreased by 47.6 kJ/mol and 46.5 kJ/mol, respectively. In 10th cycle tests, the MgH 2 + 10 wt% NiO@NiMoO 4 composite still has good cycle stability. After adding a small amount of biomass charcoal, the hydrogen storage capacity can even be maintained above 97%. Furthermore, the characterization results show that the in situ generated new species Mo and Mg 2 Ni/Mg 2 NiH 4 synergistically promote the adsorption and dissociation of hydrogen. This new synergistic mechanism provides new comprehensive insights for improving reversible hydrogen storage in MgH 2 .
研究领域:
材料科学
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能源科学
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产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Mingqiang Chen,Wei Dai,Yishuang Wang,Zhiyuan Tang,Hong Li,Chang Li,Zhonglian Yang,Jun Wang
Lignin catalytic depolymerization (LCD) into liquid fuels and aromatic chemicals in supercritical ethanol systems is one of the most effective strategies for efficient utilization of biomass resources. In this study, a series of sepiolite (SEP) supported Mo-Mn catalysts with different Mn/Mo ratios were prepared and applied to LCD. Experimental results for lignin and 2-phenoxy-1-phenyl ethanol (PP) confirmed that Mo/Mn species promoted the breakage of β-O-4 bonds, Mn additive effectively inhibited the alkylation of intermediates, and Mn/Mo ratios distinctly affected the yields of lignin oil (LO) and guaiacols. All as-prepared Mn-Mo/SEP catalysts achieved approximately 100 % conversions of lignin and PP. Various characterization results demonstrated that Mn/Mo ratios could regulate the particle sizes of metal oxides as well as the concentration of oxygen vacancies (O V ) and surface acidic sites. In 3Mn1Mo/SEP, the appropriate interaction among SEP , Mn and Mo species reduced the particle sizes of metal oxides and rendered the crystalline phase structure in a relatively complex state, which undoubtedly generated massive steps/corners on its surface and then enhanced the hydrogenation reaction. Furthermore, the 3Mn1Mo/SEP contained many O V and suitable distribution of Lewis and Brønsted acid sites, which facilitated the adsorption of oxygen-containing intermediates and further hydrogenation and deoxygenation. Therefore, 3Mn1Mo/SEP achieved 45.7 % of LO yield with an HHV of 32.31 MJ/Kg and the highest selectivity to phenols (85.61 %) and yield of guaiacols (308.9 mg/g lignin). In addition, the plausible reaction network for LCD was proposed based on the results of experiments and characterizations.
研究领域:
生物质能
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催化化学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 19
·9228-9235
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IF 9.931
Teng Wang,Rumei Jin,Xiuqi Wu,Jie Zheng,Xingguo Li,Kostya Ostrikov
A highly efficient Ni–Mo bimetallic catalyst for the hydrogen evolution reaction can be obtained from a molybdate incorporated Ni-MOF by thermal decomposition in NH3. The catalyst is composed of crystalline Ni nanoparticles doped with amorphous low valence Mo oxide encapsulated in thin N-doped carbon layers, showing excellent HER performance, featuring a very low overpotential for the HER (η20 = 58 mV), low Tafel slope (57 mV dec−1) and excellent long term stability. The catalyst apparently outperforms N-doped carbon encapsulated Ni catalysts without Mo doping, emphasizing the critical synergetic effect of Mo doping and the surface N-doped carbon thin layer on promoting the performance of Ni based HER catalysts.
研究领域:
材料科学
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催化
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Energy Technology
·
2024
·
IF 3.6
Xueli Zhang,Shan Hu,Fangyuan Zhang,Shuchen Xing,Huilin Hu,Jinhua Ye,Defa Wang
As a promising technology to mitigate global carbon emissions, photothermal catalytic CO 2 reduction remains a great challenge in increasing the conversion efficiency and regulating the product selectivity. Herein, a series of phase-separated Ni–Mo alloy catalysts for efficient photothermal CO 2 reduction with tunable CO selectivity is reported. With the increase of Mo content, the evolution rate and selectivity of CO increases. The optimal catalyst Ni 1 Mo 1 achieves 32.1% CO 2 conversion with 98.0% of CO selectivity and 71.1 mmol g cat −1 h −1 of CO evolution rate under a 300 W xenon lamp irradiation. Further increasing the Mo content reduces the CO evolution rate while maintaining the high CO selectivity. In the mechanistic study, it is revealed that the Ni–Mo alloy with an appropriate Ni/Mo ratio (e.g., Ni 1 Mo 1 ) possesses a modified electronic structure with more negative d-band center, which increases the light absorption, reduces the H 2 dissociation, and favors the CO desorption, thereby leading to efficient and selective photothermal reduction of CO 2 to CO. In this work, a viable strategy to design nickel-based catalysts is provided for efficient and selective photothermal CO 2 reduction via composition-mediated modification of electronic structure.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Caihong Wang,Weiliang Qi,Ying Zhou,Wandi Kuang,Tamil Azhagan,Tiju Thomas,Chunjie Jiang,Siqi Liu,Minghui Yang
Efficient semiconductor-cocatalyst junctions are of direct relevance to solar energy based fuel generation. Here, Ni-Mo ternary nitrides based one-dimensional hierarchical structures (In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni)) have been successfully prepared and used to achieve visible light driven H 2 evolution. Because of the metallic-like properties of the transition metal nitrides, Ni 0.2 Mo 0.8 N(Ni) as co-catalysts can promote photo-generated charge-carriers transportation/separation and decrease the overpotential of H 2 -evolution. Thus, the photocatalytic property of optimal 1 wt% In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni) exhibits a hydrogen evolution rate of 614.2 μmol g -1 h −1 , which is about 10 times as high as that of blank In 2 S 3 (61.4 μmol g −1 h −1 ). Besides, the pure Ni 0.2 Mo 0.8 N shows higher co-catalytic properties than Ni 0.2 Mo 0.8 N(Ni). This indicates that the metallic Ni (and related species) lowers the co-catalytic role of ternary nitrides. Another robust indication of this is the fact that In 2 S 3 -Ni 0.2 Mo 0.8 N nanohybrid displays about 2 times higher H 2 evolution rate than In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni).
研究领域:
材料科学
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能源化学
✓ 已验证
DOI
高影响因子
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
·
2022
·Vol. 648
·期 14
·e202200132
·
IF 1.414
Rui Pei,Xinguo Ma,Changcun Han,Zhifeng Liu,Zhengwang Cheng,Xiaoru Dong
Reducing the phase transition temperature ( T c ) of VO 2 films to achieve the application in the field of Smart Home is still a challenge. Thus, in the work, the ultra-thin VO 2 films with different Mo doping amounts were successfully prepared by an economic sol-gel method and atmosphere annealing, aiming to further investigate the mechanism of the decrease of T c . The results show that the VO 2 films with 3 at % Mo doping possess the T c of 29.5 °C. Notedly, in the as-prepared films, the maximum transmittance in the visible region ( T vis ) is 46.3 % and the solar direct transmittance ( T sol ) is 45.8 %. According to the XPS spectra, it is confirmed that the Mo doping prominently induces the valence change of V ions from +4 to +3, inhibiting the strain in the phase transition process of VO 2 films, and leading to the decrease of T c . Our work will provide a feasible solution for reducing the T c of the ultra-thin VO 2 films.
研究领域:
材料科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Yeshuang Wang,Zhelin Su,Mingxian Duan,Huiling Fan,Ju Shangguan,Chao Yang
Metal oxides-based adsorbents used for desulfurization encounter significant challenges during practical application owing to their inferior reusability and the nature of solid waste of their desulfurization products. This situation might be alleviated to some extent through a rational design of Ni–Mo composite, enabling them firstly to be used as adsorbents for H 2 S removal, and then being utilized as catalysts after desulfurization for C 4 H 4 S hydrogenation. The Ni–Mo composites before and after desulfurization were characterized using XRD, FT-IR, SEM, N 2 adsorption–desorption, XPS, CO 2 -TPD and H 2 -TPR techniques. The experimental findings suggested that Ni and Mo species function as primary active sites for H 2 S adsorption and C 4 H 4 S hydrogenation reactions, respectively. The Ni and Mo composite greatly facilitated the coupling of these two reactions due to the formation of NiMoO 4 phase. This novel active phase not only boosted the interaction between metal and H 2 S but also promoted the formation of weak and moderate alkaline sites, thereby significantly enhancing desulfurization performance. Importantly, this active phase fostered the sulfurization of Mo species and transforming into a Ni–Mo–S component, further favoring the subsequent catalytic reaction in C 4 H 4 S hydrogenation. Consequently, the prepared Ni–Mo composite oxides exhibited excellent properties in H 2 S adsorption and C 4 H 4 S hydrogenation activity, surpassing the capabilities of single metal adsorbents and commercial hydrogenation catalysts.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子