INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Peilin Wu,Lin Gao,Liuyan Dong,Zihan Lin,Lili Cui
To prepare bifunctional electrocatalyst towards HER and OER is extremely important for promoting the development of electrochemical water splitting technology. Herein, the element doping method is employed to tune the electron environment of cobalt phosphide (CoP). The Mo-doped CoP supported on carbon cloth (CC) is constructed by solvothermal and annealing method. The effect of Mo on the electron modulation of CoP during different phosphating time was studied carefully. It is noted that the Mo play an important role in tuning the electron state of Co and P elements which can trap the electron and was reduced to low valence, then transfer the electron to Co and P. With increasing the phosphating time, the electron transfer phenomenon between Mo and CoP is obvious. Benefiting from the electron engineering of Mo, Co and P as well as thin and wrinkle sheets structure, the optimal electrocatalyst only requires 39 mV and 251 mV to deliver 10 mA cm −2 for HER and OER, respectively. Also, as for the whole water splitting performance, it delivers 10 mA cm −2 at cell voltage of 1.56 V. Importantly, Faraday efficiency of the optimal catalyst achieves 99.9% for HER due to the tuned electron state of Co and P, high ECSA and low R ct .
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MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING
·
2023
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IF 6.4
Shu-Xin Yan,Guo-Dong Sun,Jian-Ping Xu,Jia Xu,Fu-Fa Wu
Simultaneous achieving the second-phase particle strengthening, high density, and fine grain is a great difficulty for designing and preparing Mo alloys . In this study, the effects of γ-Al 2 O 3 and Y 2 O 3 nanoparticles on the microstructures and properties of Mo composites prepared via spark plasma sintering (SPS) were systematically investigated. It was found that for pure Mo and Mo–Y 2 O 3 powders, Mo compact with both high density and fine grain size can't be achieved. However, Mo-Al 2 O 3 composite with both a relatively high density (98%) and a fine grain size (1.67 μm) was synthesized successfully. The small γ-Al 2 O 3 particles transformed into larger κ-Al 2 O 3 particles by obvious grain boundary migration and grain growth in the sintering process, which effectively pinned the migration of Mo grain boundary with few effects on the surface atom diffusion of Mo. Moreover, there was a crystallographic orientation relationship between the κ-Al 2 O 3 particles and Mo matrix (Mo (110)//Al 2 O 3 ( 13 4 ‾ 1 )). Ultrafine Mo composite containing dispersed Al 2 O 3 particles with stable boundary adhesion can efficiently hinder dislocation movement and crack propagation , resulting in the obvious enhancements of bending strength , hardness and compressive yield strength.
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CERAMICS INTERNATIONAL
·
2022
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IF 5.532
Yisheng Xu,Yaoheng Liang,Zeng Yuai,Hangyu Long,Qizhi He,Kaijin Guo,Yuyuan Zhang,Dongchu Chen,Xuejun Xu,Huawen Hu
Although g-C 3 N 4 (CN) materials have been extensively explored for the photocatalytic degradation of organic pollutants, their weak response to visible light and fast recombination of photoexcited electron-hole pairs restrain their practical applications. Herein, we deeply mediated the CN's energy-band structure, morphology, and surface properties by non-metal (P) and metal (Mo) co-doping based on the thermal treatment of a phosphomolybdic acid hydrate and dicyandiamide mixture in a straightforward one-step manner. Meanwhile, cyano groups and nitrogen vacancies were generated as a result of the co-doping, and the resulting P, Mo co-doped CN (PM-CN) exhibited thinner layers, smaller sizes, and superior visible-light harvesting capacity and charge separation efficiency. Consequently, highly active PM-CN was obtained for photocatalytic tetracyclines (TC) degradation, and the rate was calculated to be 0.01 min −1 , 3.3 times greater than that of the pure CN, outstripping the single P- and Mo-doped counterparts. A free radical scavenging test demonstrated that the reactive species •O 2− and h + were critical in TC degradation. The present work is expected to shed light on co-doping CN with non-metal and metal elements to obtain high-performance, visible-light-responsive photocatalysts for practical environmental remediation.
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CHEMICAL PHYSICS LETTERS
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2022
·
IF 2.719
Lifeng Han,Yuheng Liu,Chaoqun Chang,Meng Liu,Zhikun Peng,Feilong Gong
We reported the design of cactus-like Mo-WO 3 nanoarchitecture assembled of 1D nanoneedles and 2D nanosheets for achieving a highly improved NO 2 sensing performance. The nanoneedles were vertically studding between the nanosheets forming a cactus-like WO 3 nanoarchitecture, leading to highly exposed absorption sites. Mo was introduced in the WO 3 nanoarchitecture to introduce oxygen vacancy, resulting in highly activated sites. The resultant 2%Mo-WO 3 delivered the sensitivity (Rg/Ra) of 285 to 10 ppm NO 2 , which was nearly three-times higher than that of pristine WO 3 . The recovery time was only 24 s, which was greatly decreased, compared with 172 s of pristine WO 3 .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Xiaoqiang An,Li Quan,Jianqiao Liu,Qingwen Tang,Huachun Lan,Huijuan Liu
Designing non-precious electrocatalysts with multiple active centers and durability toward overall water splitting is of great significance for storing renewable energy. This study reports a low-cost Mo, Fe codoped NiCoP x electrocatalysts derived from Co-Fe Prussian blue analogue and following phosphorization process. Benefitted from the optimized electronic configuration, hierarchical structure and abundant active sites, the Mo,Fe-NiCoP x /NF electrode has shown competitive oxygen evolution reaction ( ƞ 10 = 197 mV) and hydrogen evolution reaction performance ( ƞ 10 = 99 mV) when the current density is 10 mA cm −2 in 1 M KOH solution. Moreover, the integrated water splitting device assembled by Mo,Fe-NiCoP x /NF as both anode and cathode only needs a voltage of 1.545 V to reach 10 mA cm −2 . Density functional theory results further confirm that the Mo, Fe codoped heterostructure can synergistically optimize the d-band center and Gibbs free energy during electrocatalytic processes, thus accelerating the kinetics of electrochemical water splitting. This work demonstrates the importance of rational combination of metal doping and interface engineering for advanced catalytic materials.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Wenhao Chen,Junrong Zeng,Gaowei Zhang,Jie Yu,Yejun Qiu
Developing efficient bifunctional catalysts for hydrogen and oxygen evolution reactions (HER/OER) has attracted great interest in hydrogen production from water splitting. In this work, a novel material of Mo-doped NiFe x nanospheres on 3D graphene fibers (Mo-NiFe x /3DGFs) has been successfully fabricated through a simple and cheap one-step electrodeposition method. The Mo-NiFe x /3DGFs possessed ultra-high conductivity and specific surface area, greatly benefiting to electrocatalytic hydrolysis activity. And it was found that Fe element could obviously promote OER process, while Mo doping facilitated both OER and HER reactions. We proved that there existed synergetic roles between Fe and Mo element, which could realize the control of the electronic structure and optimize the adsorption/desorption of intermediates. And electrochemical tests showed that the Mo–Ni/3DGFs exhibited a relatively smaller overpotential of 109.9 mV for HER, while the Mo-NiFe x /3DGFs presented better OER performance with an overpotential of 240.8 mV at the current density of 100 mA cm -2 in 1.0 M KOH. Finally, a system for overall water splitting constructed by Mo–Ni/3DGFs||Mo–NiFe 0.68 /3DGFs electrodes has a low cell voltage of 1.52 V at 10 mA cm −2 and long-term stability, exceeding most of literature results. Our findings provide insight into possibilities for the simple synthesis of high-performance and cheap catalysts, and laid the foundation for the practical application of transition metal catalysts .
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ENERGY & FUELS
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2022
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IF 4.654
Cheng Lan,Heping Xie,Yifan Wu,Bin Chen,Tao Liu
Electrochemical seawater splitting using efficient HER (hydrogen evolution reaction) and OER (oxygen evolution reaction) electrocatalysts have become an appropriate method for the mass production of green hydrogen. In this study, a noble-metal free OER electrocatalyst consisting of Mo-doped Ni3S2 nanocluster arrays on Nickle foam (Mo–Ni3S2/NF)─fabricated using a modified one-step solvothermal approach─is developed and evaluated. The proposed electrocatalyst demonstrates exceptional OER activity, requiring overpotentials of only 212 and 291 mV to deliver OER current densities of 10 and 100 mA cm–2, respectively, in alkaline seawater. The presence of Mo promotes Ni–S coordination, resulting in strong electronic interactions and substantially enhanced OER kinetics. Meanwhile, surface sulfate ions and (oxy)hydroxide (NiOOH) generated during the OER lead to enhanced activity and corrosion resistance, enabling Mo–Ni3S2/NF to operate continuously at 100 mA cm–2 for 500 h in alkaline natural seawater. This study is expected to inform the progression of sulfur-based transition-metal electrocatalysts for seawater oxidation.
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Biomass Conversion and Biorefinery
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2022
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IF 4.05
Chen Jiajia,Xiu Pengcheng,Gu Xiaoli
Lignin is the world’s greatest renewable aromatic biomass resource, with considerable potential for the development of high-value-added compounds. Herein, wet impregnation was employed to create Co-Mo/ATP-CZO bimetallic catalysts, which were then used to catalyze the depolymerization of lignin in ethanol and isopropanol. The findings of the characterization revealed that doping Mo metals resulted in the change of metallic oxide phase, which increased the oxygen vacancy (O V ), improved metal-carrier interaction, and decreased acid center content. The results of the experiments demonstrated that catalytic hydrogenation with a 12Mo-20Co/ATP-CZO catalyst at 240 °C for 8 h produced the maximum yield of bio-oil (57.44 wt%, including 37.58 wt% of monomer). Under these conditions, the bio-oil had a higher heating value of 33.20 MJ/kg, which was significantly higher than the alkali lignin’s 19.62 MJ/kg. Catalyst stability tests also revealed good recyclability. This research will provide an efficient method for depolymerizing lignin. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Zhiliang Jin,Teng Li,Kai Wang,Xin Guo
Simple high-temperature calcination and hydrothermal methods were followed to synthesize CeO 2 and Mo-S, respectively. The efficient photocatalytic hydrogen evolution activity exhibited by the composite catalysts can be attributed to the edge active sites in Mo-S. The Mo-O bonds formed between CeO 2 and Mo-S could further accelerate the processes of separation and migration of electrons between the catalyst interfaces. The hybrid catalyst 10%-CeO 2 /Mo-S exhibiting the best hydrogen generation ability (4.3 mmol h −1 g −1 ) was obtained by optimizing the content of CeO 2 in CeO 2 /Mo-S. Analysis of the PL spectral profile and photocurrent response recorded for the system revealed that 10%-COMS exhibited excellent photogenerated carrier separation ability. Analysis of the LSV and EIS curves revealed that 10%-COMS exhibited the optimal hydrogen production potential. The charge migration resistance provided by the systems was lower than the charge migration resistance provided by CeO 2 and Mo-S. The synergism between the S-scheme heterojunctions and the Mo-O bonds helped accelerate the separation and migration of photo-induced carriers at the catalyst interfaces. The introduction of covalent bonds in the S-scheme heterojunctions and the results presented herein can potentially help develop a new method to realize photocatalytic hydrogen evolution.
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CRYSTENGCOMM
·
2021
·Vol. 23
·期 38
·6668-6674
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IF 3.545
Xianpei Ren,Qingbo Wei,Fei Wu,Yonghua Wang,Qiang Li
Transition metal sulfides, such as molybdenum sulfide and vanadium sulfide, have recently attracted substantial attention due to their potential application to the catalysis of the hydrogen evolution reaction (HER). Alloying is one of the powerful methods to exceed the intrinsic properties of pure metals. In this study, we report a simple one-step sintering method to synthesize MoS2, V1.5S2 and V–Mo–S alloys on carbon nanotubes (CNT/VMoS). Due to its compositional, morphological and electrical superiorities, the CNT/VMoS-2 catalyst recorded the optimal HER activity with a low overpotential of −146 mV at 10 mA cm−2, a low Tafel slope of 61 mV dec−1 and a very small Rct value of 8.8 Ω, which were superior to CNT/MoS2, CNT/V1.5S2 and other CNT/VMoS catalysts in acidic media, holding a great promise for practical water-splitting applications. We believe that the present work could broaden our horizon about the preparation of other transition metal sulfide alloys and provide a platform to understand the fundamental catalytic mechanism for improving HER performance.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Yao Xu,Jack Yang,Ting Liao,Riyue Ge,Yang Liu,Jiujun Zhang,Ying Li,Mingyuan Zhu,Sean Li,Wenxian Li
Molybdenum carbide (Mo 2 C) exhibits unique competitive advantages in electrochemical water splitting due to its physicochemical properties . The high intrinsic activity is essential for the high-efficient Mo 2 C catalysts. Herein, transition metal (Ni, Co, or Fe)-Mo 2 C-embedded in N-doped carbon sheets grown on Ni foam (TM/Mo 2 C-NCSs) are synthesized to enhance the intrinsic activity of Mo 2 C by optimizing the Mo-H bonding energy through the interfacial interactions between Ni, Co, or Fe, and Mo 2 C. Owing to the superior intrinsic activity, fast ternary channels, and abundant active sites, the Ni/Mo 2 C-NCSs possess the lowest overpotential for HER (131 mV) and the Fe/Mo 2 C-NCSs show the lowest overpotential for OER (293 mV) at a current density of 100 mA cm −2 in 1 M KOH. The results analyzed with the Density function theory (DFT) calculation indicate that the most superior H adsorption site is at the interface between Mo 2 C and Ni hybrid. H was adsorbed on interface Mo&Ni@Ni/Mo 2 C with proper hydrogen adsorption free energies (ΔG H* ), achieving a fast desorption process in HER. This mechanism is absent in the pristine Mo 2 C catalysts. An alkaline electrolyzer with a cathode of Ni/Mo 2 C-NCSs and anode of Fe/Mo 2 C-NCSs demonstrates a small voltage of 1.66 V at a current density of 100 mA cm −2 . This work offers an elaborated strategy of interface engineering to enhance the intrinsic catalytic activity of Mo 2 C by accelerating H 2 desorption in HER and enhancing the catalytic kinetics of OER simultaneously.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
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IF 10.588
Yunjin Yao,Huanhuan Hu,Hongda Zheng,Hongwei Hu,Yinghao Tang,Xiaoyan Liu,Shaobin Wang
Bimetallic Fe- and Mo-embedded N-enriched porous biochar (Fe-Mo@N-BC) is developed and serves as a cost-effective and highly efficient catalyst for mineralization of non-biodegradation organic contaminants . Fe-Mo@N-BC was prepared by pyrolysis of complex Fe/Mo -containing precursors. Transmission electron microscopy and elemental mapping suggested that Fe and Mo are uniformly dispersed in nitrogen-doped biochar with hierarchical mesopores . In comparison to Fe@N-BC and Mo@N-BC, Fe-Mo@N-BC exhibited a superior activity for activating peroxymonosulfate (PMS). The stable activity was ascribed to N-doping and synergistic effect of Fe and Mo species, where both Fe-N x and Mo-N x can simultaneously serve as the active sites and N-BC can act as a carrier and an activator as well as an electron mediator. Electron paramagnetic resonance and quenching experiments indicated that H O • , O 2 • − and 1 O 2 were responsible for organic degradation . The effects of PMS dosage, initial Orange II concentration, temperature, solution pH, coexisting anions and humic acids on organic degradation were also investigated. With the assistance of an external magnet, Fe-Mo@N-BC can be easily separated after reaction and remains stable in the reusability tests. This work demonstrates a feasible strategy towards the fabrication of Fe, Mo-embedded N-enriched porous biochar catalysts for the detoxification of organic contaminants.
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