ACS Applied Energy Materials
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2020
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IF 4.473
Yin’an Zhu,Ye Pan,Weiji Dai,Tao Lu
Electrochemical splitting of water to hydrogen is widely considered as an efficient and sustainable solution to relieve the energy crisis. In this work, we report a facile dealloying method based on metallic glass (Ni61Zr36Mo3) to introduce abundant oxygen vacancies (Ov) for the electrocatalytic hydrogen evolution reaction (HER). The corroded ribbons are composed of a sandwich-like structure with Ni–Mo–O nanoporous layer outside and raw metallic glass inside. This complex structure delivers a low overpotential of 71 ± 2.6 mV at −20 mA cm–2geo in 1.0 M KOH solution, a Tafel slope of 57 ± 3 mV dec–1, and 100 h long-term stability for HER, which is much better than those of the crystallized counterpart, nanoporous Ni, and the commercial benchmark 20% Pt/C electrocatalyst. The high concentration of oxygen vacancies (71.5%), the alloying effect of Mo, and amorphous composition synergistically contribute to the superior electrocatalytic ability and enhanced reaction kinetic of nanoporous Ni–Mo–O, indicating it an excellent low-cost alternative for platinum in hydrogen production.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yichao Liang,Chao Xiong,Xiantai Zhou,Can Xue,Hongbing Ji
A Mo-based catalyst (Mo/CBC) was successfully prepared by a hydrothermal method in which the carbon support was derived from agricultural waste . Physio-chemical properties showed that Mo/CBC had uniformly dispersed particles, large pores, excellent thermal stability and high molybdenum loading. The catalytic performance was systematically investigated, including types of loading metal, oxidants, catalyst usage, substrate concentration, oxidant ratio, reaction temperature, reaction time, reusability, and scalability. Mo/CBC exhibited excellent catalytic performance in the epoxidation of 1-hexene with 98.5% of 1-hexene oxide selectivity, 94.4% of 1-hexene conversion and 99.1% of TBHP consumption efficiency under optimal reaction conditions. The catalytic performance of Mo/CBC did not decrease significantly after five cycles, showing excellent cycle stability. In addition, the scalability showed that Mo/CBC had a good universality for linear olefins, cyclic olefins, aromatic olefins and so on. Thermodynamics showed that the epoxidation system presented as an endothermic and disordered process. Kinetics study showed the rate of the reaction obeyed the pseudo-second-order model with an apparent activation energy of 75.2 kJ/mol. The mechanism study revealed that Mo 4+ species played a key role in the reaction system, promoting the generation of peroxyl radical intermediates from TBHP to directly epoxidize 1-hexene into 1-hexene oxide.
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RSC Advances
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2023
·Vol. 13
·期 50
·35689-35694
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IF 3.9
Huandi Hou,Ting Wang,Baohuan Wang,Wenting Guo,Xiang Miao,Xin Liang
Co–Mo–S based catalysts have promising applications in both the hydrogen evolution reaction (HER) and hydrodesulfurization (HDS). Herein, Co–Mo–S catalyst and Co–Mo–S catalyst with and without NaBH4 modification have been successfully synthesized by a simple hydrothermal synthesis method. Co–Mo–S catalysts with NaBH4 modification show better catalytic activity towards both HDS and the HER. The phase purity, morphology, crystal structures and electron valence distribution of the catalysts with and without NaBH4 modification were studied by experimental characterizations and theoretical calculations. The catalysts without NaBH4 modification are mostly 2H-MoS2, while the catalysts without NaBH4 modification have 1T-MoS2, and 1T-MoS2 is exposed to more active sites, which will be conducive to the results of HDS performance of the catalyst. DFT calculations investigated the required activation energies of 1T-MoS2 and 2H-MoS2 for HDS and HER, respectively. The activation energy required for both HDS and H2 generation of 1T-MoS2 is significantly lower than that for the 2H-MoS2 structure.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 27
·70884-70896
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IF 5.8
Li Ke,Zhu Yuqiu,Wang Zixuan,Chen Dingkai,Wu Wenwei,Luo Yongming,He Dedong
High concentration of H 2 S in acidic natural gas will lead to poisoning of catalysts for hydrogen production by methane steam reforming, thus limiting the further use of natural gas. Reforming CH 4 by H 2 S can be considered as an alternative route to hydrogen production from methane. This process not only achieves the removal of H 2 S but also obtains chemical raw material CS 2 and clean energy H 2 . By impregnating the Mo source on SiO 2 treated with hydrogen peroxide and then using the catalyst in the CH 4 /H 2 S reforming reaction, we surprisingly found that the conversion rate of CH 4 and H 2 S increased from 28 and 32% to 34% and 43%, respectively, after hydrogen peroxide treatment. The H 2 production rate and the yield of CS 2 increased from 20 mmolH 2 /(g Mo *min) and 52% to 30 mmolH 2 /(g Mo *min) and 65%, respectively. Combining with characterization methods such as X-ray diffraction (XRD), hydrogen temperature programmed reduction (H 2 -TPR), 1 H-based solid-state nuclear magnetic resonance ( 1 H MAS NMR), X-ray photoelectron spectroscopy (XPS), Raman spectra (RS), and transmission electron microscopy (TEM), we found that the hydroxyl concentration of the support increased after hydrogen peroxide treatment, which led to the strengthening of the force between the metal and the support, which was easy to form low-level and small-size MoS 2 , exposing more active sites, and further improving the catalytic activity. This method provides a new idea for hydrogen production by CH 4 /H 2 S reforming and the development of high-performance MoS 2 -based catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xueling Wang,Xuming Zhang,Yifan Xu,Hao Song,Xingrui Min,Zihuan Tang,Chaoran Pi,Jianping Li,Biao Gao,Yang Zheng,Xiang Peng,Paul K. Chu,Kaifu Huo
The development of earth-abundant electrocatalysts with Pt-like catalytic activity for the hydrogen evolution reaction (HER) is of great significance to green hydrogen production . Herein, a novel strategy is described to construct dual-phase nitride nanobelts composed of Mo 2 N and Ni 0.2 Mo 0.8 N by nitridation of Ni 2+ intercalated layered MoO 3 nanobelts (NBs). The Mo 2 N/Ni 0.2 Mo 0.8 N catalyst exhibits superior stability and a low overpotential of 26 mV at 10 mA cm −2 and Tafel slope of 31 mV dec −1 in both the alkaline electrolyte and simulated seawater, which is comparable to or better than that of the benchmark Pt/C catalyst. The excellent alkaline HER characteristics is attributed to the Mo 2 N/Ni 0.2 Mo 0.8 N heterostructure with adjustable content and robust interfaces and without metal Ni segregation and structure collapse during nitridation. Density-functional theory (DFT) calculations and experiments reveal that the Mo 2 N/Ni 0.2 Mo 0.8 N interface with strong electronic interactions optimizes H adsorption/desorption yielding moderately weak bonding metal sites with positive ΔG H* as the catalytic centers, thereby accelerating the HER kinetics and boosting the HER activity. The results reveal a simple strategy for the preparation of heterostructured nitride-based catalysts with Pt-like activity for hydrogen evolution.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yilong Tian,Wenhui Yi,Qiuya Shao,Minghai Ma,Lei Bai,Rundong Song,Ping Zhang,Jinhai Si,Xun Hou,Jinhai Fan
The development of nanotherapeutics that can efficiently inhibit tumors and rapidly degrade in both cured and healthy tissues remains a research imperative. Herein, we developed tumor microenvironment (TME)-responsive Mo-doped W 18 O 49 nanobundles (MoWO NBs), which are co-assembled hyaluronic acid (HA) and doxorubicin (DOX) to achieve CT/FL imaging-guided multimodal cancer therapy. MoWO NBs exhibit multiple merits: (1) MoWO NBs degrade rapidly in the normal physiological environment but slowly in the weakly acidic TME, which leads to the selective accumulation of MoWO NBs at tumor sites and can prolong the therapeutic effect. (2) The existing Mo 4+ and W 5+ ions in MoWO NBs bestow the NBs with Fenton-like reaction activity to generate cytotoxic hydroxyl radicals (OH) from endogenous H 2 O 2 . Meanwhile, overexpressed glutathione (GSH) can reduce Mo 6+ and W 6+ ions in MoWO NBs to lower valence states, further enhancing the chemodynamic activity of MoWO NBs. (3) Under NIR-II laser irradiation, MoWO with a photothermal conversion efficiency of 45.5% could trigger powerful photothermal therapeutic effects in vitro and in vivo . (4) Owing to the fluorescence emission of DOX and the high Z-elements of molybdenum and tungsten, fluorescence (FL) imaging and computed tomography (CT) imaging have the potential to be used to monitor the biodistribution of Mo-W 18 O 49 @DOX@HA (MoWODH) in vivo . More importantly, the synergistic Chemo/PTT/CDT of MoWODH NCs greatly inhibited tumor growth. This work may broaden the path for smart nanomaterials and TME-responsive therapies.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Xiaoya Yang,Xiaodan Zhang,Yuming Huang
Modulation of surface oxygen vacancies (O v ) by defect engineering is an attractive strategy for designing high performance transition metal oxide nanozymes. In this work, we reported the fabrication of the CoMoO 4 oxidase-like nanozyme, i.e. CoMo-300r, by first pyrolyzing the CoMo layered double hydroxide precursor in an air atmosphere at 300 °C and subsequent NaBH 4 reduction strategy. Various characterization outcomes confirm the mesoporous structures of both CoMo-300r and no NaBH 4 treated CoMo-300, while the specific surface area of CoMo-300 is significantly increased from 103.54 m 2 ·g −1 to 165.24 m 2 ·g −1 after NaBH 4 reduction. Also, NaBH 4 reduction treatment leads to the formation of O v rich CoMoO 4 and reduced metal ion species on the surface, promoting the redox reaction kinetics. The CoMo-300r prepared at a molar ratio of Co to Mo of 1:2, pyrolysis temperature of 300 °C and 10 mM NaBH 4 exhibited the best oxidase-like activity. The oxidase-like activity of CoMo-300r is 2.6-fold times that of no NaBH 4 treated optimal CoMo-300. The CoMo-300r can effectively promote TMB oxidation to produce blue color and has the Michaelis-Menten constant of 0.0428 mM, which was lower than most cobalt-based oxide nanozymes and indicated a higher affinity for TMB. In terms of inhibition of SO 3 2− on the CoMo-300r/TMB system, a sensitive SO 3 2− colorimetric sensing platform was established. The linear range and limit of detection for sulfite determination were 0.2–40 μM and 0.09 μM, respectively. The relative standard deviation for the determination of 10 μM sulfite was 1.41% ( n = 11). The method was successfully applied to the detection of sulfite in white wine. This work provides a new strategy to fabricate high activity oxidase mimetic for food analysis.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Cong Wang,Hongli Wang,Zhili Wang,Xiaoju Li,Yue Chi,Minggang Wang,Dawei Gao,Zhankui Zhao
Ammonia borane (AB) has been identified as one of the most promising candidates for chemical hydrogen storage . However, the practical application of AB for hydrogen production is hindered by the need of efficient and inexpensive catalysts. For the first time, we report that the incorporation of Mo into Cu@Co core-shell structure can significantly improve the catalytic efficiency of hydrogen generation from the hydrolysis of AB. The Cu 0.81 @Mo 0.09 Co 0.10 core-shell catalyst displays high catalytic activity towards the hydrolysis dehydrogenation of AB with a turnover frequency (TOF) value of 49.6 molH 2 mol cat −1 min −1 , which is higher than most of Cu-based catalysts ever reported, and even comparable to those of noble-metal based catalysts. The excellent catalytic performance is attributed to the multi-elements co-deposition effect and electrons transfer effect of Cu, Mo and Co in the tri-metallic core-shell NPs.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2024
·
IF 11.2
Xiaodong Yang,Haochen Shen,Xiaoming Xiao,Wei Yang,Zhichao Li,Na Yang,Luhong Zhang
In this work, P and Mo dual-doped CoNiS (PMo-CoNiS) nanosheet arrays were successfully constructed through a common solvothermal treatment. The precise doping of P and Mo species into the CoNiS can regulate the microstructures and meanwhile endow with PMo-CoNiS abundant amorphous/crystalline heterointerfaces, which can adjust the electronic structure, thus enhancing the intrinsic activity of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). As a result, ultra-low overpotentials of merely 156 and 58 mV are required to deliver a current density of 10 mA cm −2 for OER and HER, respectively, and the electrocatalysts PMo-CoNiS also exhibit low Tafel slopes and maintain robust stability for 48 h in alkaline media at a high current density of 50 mA cm −2 . In addition, in an assembled electrolyte cell for overall water splitting, a voltage as low as 1.48 V is sufficient to yield a current density of 10 mA cm −2 . Density functional theory (DFT) calculations further confirmed that the enhanced OER and HER result from the optimized OH* and H* adsorption energy of PMo-CoNiS due to P, Mo dual doping and generated interfacial effect. This work may offer an avenue for designing low-cost bifunctional catalysts with superior catalytic activity and provide a new application strategy for broader applications in various electrocatalytic fields.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Jianmin Li,Changyan Guo,Yanan Niu,Xianglei Cao,Jiang Li,Jide Wang
The photocatalytic oxidation of benzyl alcohol and the simultaneous evolution of hydrogen from water are efficient dual-optimal routes. It is important to develop composite catalysts that combine redox properties and facilitate electron–hole separation and transport. Herein, the bimetallic-doped Mo-ZIS@Ti photocatalyst was designed and synthesized, and the selective oxidation of benzyl alcohol and hydrogen evolution by water splitting was realized at the same time. Under visible light irradiation, benzyl alcohol was completely converted with more than 99% selectivity for benzaldehyde, and the H2 production rate was 5.6 times higher than the initial ZIS. The exceptional catalytic performance was ascribed to utilizing Ti-MIL-125 as a precursor, wherein slowly releasing-doped Ti formed robust Ti–S bonds that quickly transfer electrons and reduce sites. Meanwhile, doping Mo effectively captures photogenerated holes and acts as active sites for oxidation reactions. Both experimental characterization and work function calculations demonstrate that the bimetallic synergism effectively modulates the electronic structure of ZIS, promotes the directional separation of electrons and holes, and significantly improves the photoactivity and stability of ZIS. This work contributes a route to obtain benzaldehyde and green hydrogen at the same time and also gives new insights for the construction and mechanism study of bimetallic-doping catalysts.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Daming Feng,Lixue Zhou,Chang Liu,Hui Li,Yusheng Zhang,Yali Yao,Tianyi Ma
Electrocatalytic nitrogen reduction reaction (NRR) for the synthesis of ammonia (NH 3 ) is one of the green and mild methods of artificial nitrogen fixation, promising as an alternative to replace the existing industrial process. Under the requirements of green chemistry and sustainable development, the design and development of highly active and stable electrocatalysts is very important for improved synthesis performance. Mimicking from the natural nitrogenase, Fe and Mo based catalysts have attracted much attention due to their superior catalytic performance for N 2 adsorption and activation. In this work, an interfacial engineering strategy has been used to prepare a Fe, Mo-bimetallic electrocatalyst for the electrosynthesis of NH 3 . In detail, the pre-pyrolyzed biochar-based Fe 2 O 3 composites were decorated with nano-flowered MoS 2 /MoO 2 hybrids by a solvothermal process (MoS 2 /MoO 2 @Fe 2 O 3 /BC). As confirmed by the extensive characterization, the further modification not only introduced functional counterparts into the electrocatalysts but also regulated the morphology of the nanostructure. The electrochemical tests showed that the highest NH 3 yield rate of MoS 2 /MoO 2 @Fe 2 O 3 /BC was 4.87 μg h − 1 cm −2 and highest FE was 16.5% in 0.1 M Na 2 SO 4 . The catalytic stability and durability were also presented in the longtime electrolysis and cycling experiments. The improved catalytic performance of decorated catalyst, as evidenced by the comparison with Fe 2 O 3 /BC, is attributed to the increased electrocatalytic active area, the moderated hydrophilicity, and the synergistic effect of Fe, Mo-bimetallic active sites. This study provides a new perspective for the design and development of low-cost transition metal complexes as electrocatalysts for nitrogen reduction reactions.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Qingxiang Kong,Yulei Li,Hang Ma,Qin Zhao,Linjing Yang,Ruidong Xu,Hong Guo
Hydrogen energy as a new type of clean energy has been widely used. Electrolysis is a highly effective method of producing hydrogen from water. Catalysts with low development costs and high efficiency are the focus of current research. A novel Ni–W–P/Mo catalyst for hydrogen evolution reaction (HER) was synthesized by electrodeposition based on a molybdenum mesh. The experimental results show that when the current density is 10 mA/cm2, the best overpotential of Ni–W–P/Mo in alkaline medium is 75 mV. Not only that, the Tafel slope (77 mV/dec) also proves its excellent dynamic performance. In addition, the 60 h stability test at a current density of 10 mA/cm2 indicates an excellent long-term stability performance. Compared with the catalysts reported in recent years, the HER performance of Ni–W–P/Mo is much better than that of most nonprecious metal catalysts. The uniform and regular molybdenum network provides a large area of support for the catalyst, which is conducive to the synthesis and reaction of the catalyst. By doping W, the electronic structure of the catalyst is regulated, and the water decomposition is promoted. The stability of the morphology is also an important factor in improving the activity of the catalyst. The amorphous catalyst synthesized by the electrodeposition method in this work provides a new idea for the research of catalytic materials for hydrogen production by electrolysis of water and has important significance for promoting the development of a hydrogen energy economy.
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