CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Weiwei Han,Yang Qian,Fan Zhang,Yi He,Ping Li,Xingwang Zhang
The application of proton exchange membrane water electrolysis (PEMWE) is largely limited by the sluggish oxygen evolution reaction (OER) kinetics, which usually requires noble metal Ir/Ru-based catalysts. It’s desirable to design low-cost catalysts with less content of Ir/Ru in OER without sacrificing their catalytic performance. Herein, the ultrasmall IrO 2 nanoparticles uniformly dispersed on Co 3 O 4 -CoMoO 4 nanocages (IrO 2 @Co 3 O 4 -CoMoO 4 ) electrocatalyst is demonstrated. Structural characterization indicates that hollow Co 3 O 4 -CoMoO 4 acts as the effective support to provide abundant anchoring sites and heterogenous interfaces, which enable the catalyst to expose more active sites and accelerate charge transport. As a result, the representative IrO 2 @Co 3 O 4 -CoMoO 4 exhibits an outstanding OER activity ( η = 236 mV at 10 mA cm −2 ) with a superior mass activity of 713 A g –1 Ir at 1.53 V vs. RHE in 0.5 M H 2 SO 4 that are comparable to most reported catalysts. Theoretical calculations also reveal that the introduction of Mo can effectively modify electronic structure and decrease adsorption energy barriers of oxygen intermediates, and thereby enhancing OER catalytic activity. This work provides a new idea to develop highly efficient low Ir catalysts for OER.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Jiayu Li,Jun Xiong,Haoxue Huang,Mei Zhang,Wenshuai Zhu,Jun Di
The non-stoichiometric structure of tungsten oxide (W 18 O 49 ) makes it easy to form oxygen vacancies near the low-valence W atoms, so the W 18 O 49 can be applied to oxidative desulfurization. To further improve the desulfurization activity of W 18 O 49 to meet the increasingly stringent environmental requirements, Mo doping and plasma-induced surface reconstruction cooperative strategies are developed. The incorporation of Mo species into the W 18 O 49 surface by replacing W sites can adjust the atomic and electronic structure of the catalyst surface and form more oxygen vacancies. After Mo doping into the W 18 O 49 , the plasma bombarded the surface of material to destroy part of the surface structure, thus producing the reactive sites with low coordination numbers. This reconstructed atomic surface also accompany to generate more oxygen vacancies, thus greatly improving the catalytic activity. Compared to pure W 18 O 49 , significantly improves oxidative desulfurization performance can be achieved over Mo-W 18 O 49 -P, and deep desulfurization is realized within 3 h. Moreover, the optimal Mo-W 18 O 49 -P shows better stability than pure W 18 O 49 , which can be recycled for 12 times. This work provides an accessible pathway for cooperative enhancing the catalytic oxidative desulfurization activity of oxide catalysts.
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ChemSusChem
·
2023
·Vol. 16
·期 17
·e202300633
·
IF 8.4
Wen Guo,Tao Yang,Hongyan Zhang,Hao Zhou,Maoshuai He,Wenxian Wei,Wenjie Liang,Yilin Zhou,Tingting Yu,Hong Zhao
Graphical A thick Ni-based catalyst layer derived from nickel foam was synthesized by a Fe 3+ -induced strategy. In addition to the remarkable conductivity, high stability and more accessible active sites, Mo,Fe co-modulation also optimizes the adsorption free energies of the OER intermediates, boosting the catalytic activities. A highly active catalyst for the oxygen evolution reaction (OER) is critical to achieve high efficiency in hydrogen generation from water splitting. Direct conversion of nickel foam (NF) into nickel-based catalysts has attracted intensive interest due to the tight interaction of the catalysts to the substrate surface. However, the catalytic performances are still far below expectation because of the problems of low catalyst amount, thin catalyst layer, and small active area caused by the limitations of the synthesis method. Herein, we develop a Fe 3+ -induced synthesis strategy to transform the NF surface into a thicker catalyst layer. In addition to the excellent conductivity and high stability, the as-prepared FeMo-Ni 2 P 2 O 7 /NF catalysts expose more active sites and facilitate mass transfer due to their thicker catalyst layer and highly dense coral-like micro-nano structure. Furthermore, the Mo, Fe co-modulation optimizes the adsorption free energies of the OER intermediates, boosting catalytic activities. Its catalytic activity is among the highest, and it exhibits a small Tafel slope of 34.71 mV dec −1 and a low overpotential of 161 mV for delivering a current density of 100 mA cm −2 compared to reported Ni-based catalysts. The present strategy can be further used in the design of other catalysts for energy storage and conversion.
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PubMed
高影响因子
ChemNanoMat
·
2023
·Vol. 9
·期 7
·e202300087
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IF 3.8
Tingyi Wu,Huanglin Dou,Zhenxin Zhao,Junliang Zhou,Xiaomin Wang
Graphical The NiMoO 4 -modified separator can not only use its own strong polarity to chemisorption of polysulfides and effectively suppress the shuttle effect, but also can promote the mutual transformation between polysulfides of different phases, reduces the reaction potential barrier, and the redox kinetics is significantly improved. Besides, the hollow microsphere structure facilitates the penetration of electrolyte and establishes a pathway for ion/electron transport, which accelerates the Li + diffusion rate. Lithium-sulfur (Li−S) batteries are considered to be the most promising candidates for achieving low-cost, high-energy density systems. The serious shuttle effect of polysulfides (LiPS) and the sluggish redox kinetics have become major obstacles to the practical application of Li−S batteries. Herein, a hollow microsphere structure of transition bimetallic oxide nickel molybdate (NiMoO 4 ) was prepared by hydrothermal reaction and calcination method. It was used as a separator coating material to inhibit LiPS shuttle and promote efficient redox conversion of sulfur species. The hollow microsphere structure not only possesses a large internal space to physically confine LiPS but also exposes abundant active sites to enhance the redox kinetics of LiPS. The NiMoO 4 shows superior adsorption ability for LiPS and accelerated ion/electron transport rates compared to NiO, thus facilitating the anchoring-conversion-diffusion processes of polysulfides. Benefiting from this versatility, the Li−S batteries with NiMoO 4 -PP exhibit a high discharge specific capacity of 1354.5 mAh g −1 at 0.1 C. In addition, the battery exhibits excellent cycling stability with a capacity decay rate of 0.027% for 500 cycles at 2 C. These results demonstrate the potential application of NiMoO 4 -based electrocatalysts in high-performance Li−S batteries.
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Science Bulletin
·
2023
·
IF 18.9
Guangxun Sun,Dongyuan Liu,Min Li,Shu Tao,Zekun Guan,Yanfei Chen,Shihuan Liu,Qingzhou Du,Han Guo,Xinyue Yuan,Xinying Zhang,Houyu Zhu,Bin Liu,Yuan Pan
Development of efficient catalysts with high atomic utilization and turnover frequency (TOF) for H 2 activation in slurry phase hydrocracking (SPHC) is crucial for the conversion of vacuum residue (VR). Herein, for the first time, we reported a robust and stable single atoms (SAs) Mo catalyst through a polymerization-pyrolysis- in situ sulfurization strategy for activating H 2 in SPHC of VR. An interesting atomic coordination structural dynamic evolution of Mo active sites was discovered. During hydrocracking of VR, the O atoms that coordinated with Mo were gradually replaced by S atoms, which led to the O/S exchange process. The coordination structure of the Mo SAs changed from pre-reaction Mo-O 3 S 1 to post-reaction Mo-O 1 S 3 coordination configurations, promoting the efficient homolytic cleavage activation of H 2 into H radical species effectively. The evolved Mo SAs catalyst exhibited robust catalytic hydrogenation activity with the per pass conversion of VR of 65 wt%, product yield of liquid oils of 93 wt%, coke content of only 0.63 wt%, TOF calculated for total metals up to 0.35 s −1 , and good cyclic stability. Theoretical calculation reveals that the significant variation of occupied Mo 4d states before and after H 2 interaction has a direct bearing on the dynamic evolution of Mo SAs catalyst structure. The lower d -band center of Mo-O 1 S 3 site indicates that atomic H diffusion is easy, which is conducive to catalytic hydrogenation. The finding of this study is of great significance to the development of high atom economy catalysts for the industrial application of heavy oil upgrading technology .
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Sustainable Energy & Fuels
·
2023
·Vol. 7
·期 4
·977-985
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IF 5.6
Tingting Wen,Limin Wang,Yaqiong Gong
Design and synthesis of a highly efficient OER catalyst is the key to improve the efficiency of hydroelectrolysis for hydrogen production. In this paper, a rational approach to improve the catalytic performance of CoMoO4 nanomaterial was reported. A nanoflower structured CoMoO4 precursor was synthesized on nickel foam using a typical hydrothermal method. Then, CoMoO4/NF was etched through brief immersion in iron nitrate solution at room temperature to produce FeOOH–CoMoO4/NF. The unique 3D structure of FeOOH–CoMoO4/NF could availably promote interfacial electron transfer as well as effectively provide abundant active sites, and it exhibited excellent electrocatalytic activity. FeOOH–CoMoO4/NF requires an overpotential of 209 mV to achieve a current density of 10 mA cm−2. Meanwhile, the material FeOOH–CoMoO4/NF exhibits excellent catalytic durability of up to 24 h, which is promising for practical applications in energy conversion. Thus, this work may offer a viable strategy to assemble remarkable OER electrocatalysts.
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APPLIED SURFACE SCIENCE
·
2018
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IF 4.439
Sijie Xie,Zhijie Bi,Yongbo Chen,Xiaoli He,Xiangxin Guo,Xiangdong Gao,Xiaomin Li
Amorphous Mo-doped WO 3 films are successfully synthesized via an electrodeposition method. In comparison with the reported time-consuming and costly techniques involving heating or vacuuming steps, the proposed electrodeposition method achieves the preparation of Mo-doped WO 3 in a simple and economic all-solution route. By optimizing the dopant concentration of Mo, the as-prepared 2 at% Mo-doped WO 3 film exhibits excellent electrochromic and energy-storage properties with large optical modulation of 83.3% at 633 nm and high pseudocapacitance of 117.1 mF cm −2 (334.6 mF g −1 ), greatly superior to those of pure WO 3 films. These great electrochemical properties could be attributed to the amorphous state and the proper structure distortion caused by doped atoms. Furthermore, bifunctional devices on various substrates contained the 2 at% Mo-doped WO 3 films are demonstrated with satisfactory electrochromic and energy-storage properties as well, indicating the practical applications of the Mo-doped WO 3 films in both energy-saving and energy-storage fields.
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CATALYSIS LETTERS
·
2025
·Vol. 155
·期 2
·1-15
·
IF 2.4
Li Ziyuan,Luo Mingsheng,Yang Zhi,Cui Xiaoteng,Yang Wenshuai,Xia Lingman,Shao Changke,Rahman Roshni
To effectively mitigate the global warming issue, it is crucial to develop advanced technologies that can significantly reduce carbon dioxide emissions. CO 2 hydrogenation for methanol synthesis is increasingly recognized as a promising chemical approach for the green-house gas utilization. In this study, we present a highly active, selective and stable Mo modified ZnCu-MOF and ZnCuAl-LDH composite catalysts, which achieves 18% CO 2 conversion and 70% methanol selectivity at 230 °C, 3.0 MPa at a space velocity of 3600 mL·g cat −1 ·h −1 . Furthermore, after 140 h of operation, the catalyst demonstrates superior durability. In-situ DRIFT results reveal that this CO 2 hydrogenation reaction over the ZnCu-MOF and ZnCuAl-LDH composite catalysts proceeds through key intermediate formate species, ultimately leading to the methanol formation. In contrast, the Mo-modified catalysts facilitate the CO insertion reaction (CO 2 → CO*, CO* + *CH x → CH 3 OH), thereby enhancing the methanol yield. Graphical
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2017
·
IF 3.133
Shu Huang,Min Zhou,Kangli Wang,Shijie Cheng,Guoping Yan,Kai Jiang
Electrochemical synthesis method is an effective, controllable and cost-effective synthesis route for fabricating various kinds of metal compounds. Here, for the first time, we synthesis the Li-Mo-O compounds by electrolysing MoO 3 in molten LiCl-LiBr salt at 600 °C. The as-prepared LiMoO 2 and Li 2 MoO 4 were evaluated as novel anode materials for lithium ion batteries (LIBs), delivering high reversible capacities of 565 and 473 mAh g −1 , respectively. More significantly, the LiMoO 2 @C show extra high initial columbic efficiency of 80% with superior rate capability and long cycling stability over 200 cycles. This facile and green electrochemical synthesis route described in this work can provide new insights for the development of promising host materials for practical LIBs in large-scale energy storage applications.
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ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Mao Zhou,Ruizhuo Ouyang,Yuhao Li,Yuqing Miao
3D microspheres from the in situ synthesis, growth and organization of Ni-Mo-S nanoparticles (NPs) on porous Ti plate were obtained through a typical hydrothermal method . The Ni-Mo-S/Ti electrode exhibited excellent electrocatalytic performance for hydrogen evolution reaction (HER) in strong acid electrolyte. HER occurs at the relatively low onset potential of −4 mV with high current of 10 mA/cm 2 at low overpotential of 30 mV in 0.5 M H 2 SO 4 . Furthermore, the Ni-Mo-S/Ti exhibited excellent electrocatalytic stability over an extended period of 60000 s without obvious current decrease observed. The multinary composition , 3D microsphere-like structure from nanoparticles, porous supporting substrate, the good conductivity of Ti and good electron transfer between electrode and catalysts, all of them are combined to contribute to the high HER electrocatalytic activity of the Ni-Mo-S/Ti. The good stability comes from the stability of catalysts and Ti themselves, and the tight contact between catalysts and supporting electrode.
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JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
IF 5.3
Yong Zeng,Yingdi Dong,Xiongxing Zhang,Zhongbao Hua,Xiqing Wu,Wei Sun,Haisheng Han,Li Wang,Honghu Tang
In the flotation separation of Mo-Pb bulk concentrate and the purification process of Pb-containing molybdenite concentrate, depressants are typically added to depress galena or molybdenite, aiming to obtain high-quality flotation products. Previous studies have focused on the depression of galena. In this study, gallic acid (GA) was utilized as a molybdenite depressant during Mo-Pb flotation separation. Single mineral flotation experiments showed that pH notably influenced galena and molybdenite flotation with GA, particularly at pH 10, displaying the most substantial recovery difference. Mixed mineral flotation experiments revealed GA’s selective depression on molybdenite. At the optimal dosage of GA, the Mo recovery was reduced by 76.62 percentage points, while the Pb recovery remained unaffected. The depression and separation mechanisms of GA were investigated using contact angle, infrared spectroscopy, Zeta potential, inductively coupled plasma optical emission spectrometer (ICP-OES), X-ray photoelectron spectroscopy (XPS) analysis, first-principles calculations analysis, and interface interaction free energy calculations. The results indicate that GA treatment significantly reduces the hydrophobicity of molybdenite surfaces; however, it slightly enhances the hydrophobicity of galena surfaces. At pH 10, the primary species in GA solution is HGA 3- . It adsorbs on PbO species of the galena surface as Pb-GA complexes and tends to detach from the surface at high adsorption capacity, resulting in galena not being depressed by GA. Differently, GA adsorbs on the molybdenite surface through hydrophobic attraction force, rendering it hydrophilic. Additionally, after treatment with potassium butyl xanthate (PBX), the hydrophobicity of GA-treated galena is significantly enhanced, while the hydrophobicity of GA-treated molybdenite is not restored. This is because PBX can adsorb stably on GA-treated galena, but its adsorption on GA-treated molybdenite is hindered by the pre-adsorbed GA.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Yue Liu,Chunkai Wang,Ding Ma,Mengge Li,Yuting Sun,Xiaofei Sun,Yan Zhu,Bin Yao,Yongfeng Li,Zhanhui Ding
It is proved that secondary phases, such as Cu 2 Se, and ZnSe etc., and MoSe 2 layer can form at Cu 2 ZnSn(S,Se) 4 (CZTSSe)/Mo electrode interface, due to that Mo electrode reacts with CZTSSe and Se vapor during selenization process. The secondary phases and MoSe 2 with inappropriate thickness can decrease power conversion efficiency (PCE) of CZTSSe solar cell. In this work, a simple method was proposed to suppress the reaction between CZTSSe and Mo, and to optimize the thickness of MoSe 2 . This was achieved by growing a layer of Mo oxide in situ on the Mo electrode surface through soaking the Mo electrode in H 2 O 2 . The Mo oxide layer consisted of MoO 3 , MoO x and MoO 2 . It could suppress the reaction between Mo and CZTSSe, thus preventing the formation of secondary phases in CZTSSe. By further tuning the soaking time, the thickness and density of the Mo oxide layer were optimized, resulting in an optimized thickness of the MoSe 2 layer and a significant improvement in the contact quality at both the front and back interfaces. This improvement is beneficial for suppressing carrier recombination and reducing contact resistance. Furthermore, the Cu/(Zn+Sn) ratio in CZTSSe was optimized, leading to an expansion of the depletion region width. As a result, the reverse saturation current density and series resistance decrease, while the photogenerated current density increases. This ultimately led to a rise in PCE from 7.66% for CZTSSe solar cells with Mo electrodes that were not soaked to 8.95% for those with Mo electrodes soaked for 20 s.
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