JOURNAL OF CATALYSIS
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2025
·
IF 6.5
Jundao Wu,Zeai Huang,Zhen He,Rustem Zairov,Xiaoting He,Yue Huang,Mengyao Fu,Chengdong Yuan,Oleg G. Sinyashin,Ying Zhou
The catalytic methane(CH 4 ) and hydrogen sulfide(H 2 S) reforming (H 2 SMR) represents a promising approach for producing high-value sulfur-carbon compounds and hydrogen without generating the greenhouse gas of CO 2 . Despite its significant potential, the mechanistic understanding of interactions between CH 4 and H 2 S remains contentious, posing substantial challenges for catalyst development. In this study, we employed a Mo/Al 2 O 3 catalyst to elucidate synergistic conversion pathways between CH 4 and H 2 S during H 2 SMR. At 1173 K with a reaction duration of 0.5 h, conversion rates of CH 4 and H 2 S reached 63.7 % and 59.2 %, respectively, accompanied by H 2 and CS 2 production rates of 688.8 μmol g −1 min −1 and 444.3 μmol g −1 min −1 , respectively. Notably, the catalyst exhibited stable performance over 5 h without significant deactivation, in contrast to pure methane cracking reactions where CH 4 conversion rapidly declined from 43.6 % to 14.3 %. Through in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) combined with alternating CH 4 /H 2 S exposure experiments, we successfully tracked the synergistic conversion pathway on the Mo/Al 2 O 3 catalyst. These investigations revealed that the formation of CH 3 S intermediates serves as a critical step facilitating CS 2 generation. This mechanistic insight not only advances fundamental understanding of H 2 SMR reaction pathways but also provides a rational foundation for designing optimized catalysts with enhanced stability and extended operational lifetimes. The identification of this intermediate-driven mechanism addresses previous controversies regarding CH 4 -H 2 S interactions and offers strategic guidance for developing efficient sulfur-resistant catalytic systems.
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高影响因子
JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2016
·Vol. 16
·期 12
·12635-12639
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IF 1.338
Du Jingjing,Xie Shaowen,Li Na,Xu Jianxiong,Xu Lijian
Hierarchical nanoporous Al–SiO2 particles were prepared in this study by dissolving template method. The hierarchical nanoporous Al–SiO2 particles with hollow structure were analyzed by transmission electron microscope (TEM), energy dispersive spectrometer
(EDS), scanning electron microscope (SEM), nitrogen adsorption stripping curves and Barrett-Joyner-Halenda (BJH) pore size distribution curves. Hierarchical nanoporous Al–SiO2/Ni–Mo composite electrodes were prepared by composite deposition of hierarchical nanoporous
Al–SiO2 particles onto electroplating bath of Ni–Mo. Results showed that the specific surface area for the hierarchical nanoporous Al–SiO2 sample was 396 m2/g, with pore volume being 1.37 cm3/g and mesoporous pore size being 3.3
nm. The hydrogen evolution electrocatalytic activities for the composite electrodes reached the optimal value when the concentration of the hierarchical nanoporous Al–SiO2 in the electroplating bath was 2 g/L, indicating that their “foam” structure did not only
enhance the electrode surface area but also effectively improved the electrocatalytic properties of aluminum and showed that the electrocatalytic hydrogen evolution by the hierarchical nanoporous Al–SiO2/Ni–Mo composite electrodes had more advantages than that of the
Ni–Mo electrodes alone.
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JOURNAL OF THE ENERGY INSTITUTE
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2021
·
IF 6.186
Hao Xu,Xing Fan,Guo-Sheng Li,Yang-Yang Xu,Wen-Long Mo,Peter N. Kuznetsov,Feng-Yun Ma,Xian-Yong Wei
Co-Mo/γ-Al 2 O 3 bimetallic catalyst was prepared by incipient wetness impregnation and the physicochemical properties were obtained by a series of characterization methods. The active components are mainly MoS 2 and Co-Mo-S existing on γ-Al 2 O 3 , the support. Meanwhile, the activity of catalyst in hydroconversion of four coal-related model compounds (CRMCs), dibenzyl ether, furan, thiophene and quinoline, was investigated. Hydroconversion products were analyzed by gas chromatography/mass spectrometry (GC/MS) and the possible reaction pathways were proposed according to the GC/MS data. Oxygen was removed from dibenzyl ether via the direct cleavage of C alk -O bridge bond to produce benzylium cation followed by the combination with H − to generate toluene. The hydroconversion of furan can be realized by the direct cleavage of C ar -O bond and direct hydrogenation, respectively. For thiophene, H + directly transferred to sulfur atom, leading to the cleavage of C ar -S bond to produce H 2 S and 1,3-butadiene, which abstracted active hydrogen to yield butane. Another indirect desulfurization pathway for thiophene is hydrogenating to form tetrahydrothiophene and C–S bond cracking to produce butane. Hydroconversion of quinoline started with either N-ring or benzene ring , and the first one was the main pathway.
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高影响因子
FUEL
·
2025
·
IF 7.5
Xin Zhang,Xiangyun Sun,Li Li,Xinli Zhang,Ao-Bing Wang,Huijuan Xu,Lijun Gao,Yaohui Gao,Hui Liu
Developing low-cost, highly efficient and stable non-noble metal-based electrocatalysts for the hydrogen evolution reaction (HER) is crucial for promoting large-scale alkaline water electrolysis. Here, we report a novel self-supporting Ni(OH) x /Mo-Ni 3 S 2 nanosheet heterostructure grown on nickel foam, demonstrating outstanding catalytic performance for alkaline HER. This heterostructure electrocatalyst exhibits an exceptionally low overpotential of just 33 mV at a current density of 10 mA cm −2 in 1 M KOH solution, surpassing commercial Pt/C catalyst. Moreover, it can operate continuously for 300 h at a high current density of around 130 mA cm −2 . Both experimental and theoretical calculations show that strong electronic coupling at the heterojunction interface optimizes the adsorption energy of molecular water and hydrogen on active sites, thereby enhancing the intrinsic activity. This work offers novel insights for designing high-performance alkaline HER electrocatalysts through coupling doping and heterostructure engineering.
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高影响因子
Processes
·
2025
·Vol. 13
·期 8
·2594
·
IF 2.8
Tao Shi,Xiaoling Huang,Zhan Zhao,Zizhen Li,Kelei Huang,Xiangchao Meng
Electrocatalytic water splitting has been demonstrated to be a highly efficient and promising technology for green hydrogen production. However, the inefficiency and instability of the cathode hinder its wide application in water electrolysis. Herein, we report a rapid Joule heating method for synthesizing the Ru-Mo oxide catalyst. Comprehensive characterization results confirmed that the as-prepared catalyst featured an internal porous structure with low crystallinity, which weakened the strength of Ru-H bonds through structural and electronic modulation. The enhanced HER performance was attributed to the incorporation of Mo4+species, which strengthened Ru-O-Mo interactions. As tested, the optimized catalyst exhibited ultralow overpotentials (25.08 mV and 120.52 mV @ 10 and 100 mA cm−2, respectively) and excellent stability (100 h @ 100 mA cm−2) in a 1 M KOH solution. Meanwhile, the as-prepared catalyst was equipped in an anion exchange membrane (AEM) alkaline water electrolyzer, which could deliver 185 mA cm−2at only 2.16 V with 100% Faradaic efficiency. This study provides a feasible strategy for constructing highly efficient low-crystallinity electrocatalysts.
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PHYSICA STATUS SOLIDI A-APPLICATIONS AND MATERIALS SCIENCE
·
2025
·Vol. 222
·期 15
·2500353
·
IF 1.9
Xia Deng,Laijun Liu,Jungu Xu
The K 2 ZnV 2 O 7 material, as reported in our previous work, undergoes a phase transition from melilite-related structure to typical melilite structure upon Ga doping on the Zn site, with interstitial oxygen introduced and accompanied by an approximately two orders of magnitude ionic conductivity improvement (≈1.01 × 10 −1 S cm −1 at 600 °C for K 2 Zn 0.7 Ga 0.3 V 2 O 7.15 ). Herein, in order to further enhance the oxide-ion conduction by introducing more interstitial oxygen into the structure, a series of Ga and Mo codoped K 2 Zn 1- x Ga x V 2- y Mo y O 7+0.5 x +0.5 y (0 ≤ x ≤ 0.2, y = 0.1 and 0.2) materials are designed and synthesized via the traditional solid-state reaction method, with their phases and electrical properties being systematically studied. The results reveal that the Ga and Mo codoped materials retain the melilite-related structure and show a much lower conductivity, e.g., only ≈1.49 × 10 −2 S cm −1 at 600 °C for the composition of K 2 Zn 0.8 Ga 0.2 V 1.8 Mo 0.2 O 7.2 , despite its higher interstitial oxygen concentration compared to the single Ga-doped K 2 ZnV 2 O 7 (e.g., K 2 Zn 0.7 Ga 0.3 V 2 O 7.15 ). Therefore, the introduction of Mo into the structure appears to suppress the phase transition and decrease the mobility of interstitial oxygen for the K 2 ZnV 2 O 7 -based materials. These findings provide a more comprehensive perspective on the oxide-ion conduction optimization of melilite or melilite-related materials.
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Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 11
·6065-6072
·
IF 12.732
Junxiao Chen,Xue Fang,Zhouhong Ren,Weiye Qu,Xiaolei Hu,Zhen Ma,Liwei Chen,Xi Liu,Yaxin Chen,Xingfu Tang
Selective catalytic reduction (SCR) of NOx with NH3 has been widely used for NOx emission control, but commercial catalysts inevitably suffer severe deactivation in SO2-containing stack gases at low temperatures because the ammonium bisulfate (NH4HSO4, ABS) formed in SCR blocks the surface active sites. We resolve this issue by developing a TiO2-supported single-atom Mo catalyst (Mo1/TiO2) that decomposes ABS at ∼225 °C, far lower than the dew point of ABS (∼260 °C). Single Mo atoms paired with the neighboring surface Ti atoms function as Mo–Ti acid–base dual sites, which respectively adsorb the NH4+ and HSO4− of ABS. After the oxidation of NH4+ by surface lattice oxygen on the Mo sites, electrons left behind on the dual sites are localized around the Fermi level, which allows them to transfer to the adsorbed HSO4− on the Ti sites, thus releasing SO2 at low temperatures. The Mo1/TiO2 catalyst with Mo–Ti acid–base dual sites enables the decomposition of ABS at low temperatures, and thus this work provides a way to effectively control NOx emission particularly from industrial boilers.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Yue Du,Jiacheng Hu,Yongxu Jin,Yisi Liu,Qiyun Pan,Kai Wang,Lina Zhou,Zhenhui Liu,Xiaodi Du
The development of fast and high yield route for large scale synthesis porous TiO 2 based catalyst has attracted widespread concern in the field of optoelectronic and catalysis. Up to now, the facile synthesis of mesoporous TiO 2 based composite is still limited to wet chemical synthesis approach (hydrothermal, phase transformation, or sol-gel method etc.). Here, we develop a polyethyleneimine-assisted solvent-free strategy to synthesize of ionic liquid-derived Mo-based mesoporous TiO 2 composite, with molybdenum sites uniformly distributed on TiO 2 matrix. As-synthesized ionic liquid-derived mesoporous MoO x /TiO 2 composite is composed of uniform nano-sized anatase particles and connected by worm-like mesoporous channel. Moreover, the calcination conditions and loading amount of molybdenum-containing ionic liquid have been further optimized. These distinct characteristics endow the prospective MoO x /TiO 2 composite with excellent performance in catalytic oxidation reaction, which can remove refractory organic sulfur compound in the model fuel effectively. Our work opens a new solvent-free avenue to synthesis porous metal based ionic liquids/TiO 2 composite.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Hengyuan Liu,Yingzhe Liu,Xuecheng Zeng,Xude Yu,Jianhong Xu
Electrocatalytic nitrogen reduction reaction (ENRR) is emerging as a promising routine for the sustainable production of ammonia. Hindered by the strong triple bond in N2 and unfavorable hydrogen evolution reaction, it is critical to develop efficient catalysts with excellent activity and selectivity. Herein, we propose a novel microfluidic platform that achieves the continuous synthesis and morphology regulation of a two-dimensional heterocatalyst FeMo/g-C3N4 through a precipitation process in a confined space. Owing to the rapid mixing and microfluidic manipulation, FeMo/g-C3N4 maintains an overwhelmingly favorable structure compared to the batch methods. Benefiting from the ultrasmall active sites (0.86 nm), homogeneous nanodot distribution, and abundant 2D surface, the promoted N2 chemisorption and competitive ENRR performance can be simultaneously ensured, as confirmed by the experimental studies. By varying the applied working potential, the optimal ammonia yield can be determined as 33.25 μg h–1 mgcat.–1 at −1.2 V. This work innovatively opens a pathway for morphological fine structural tuning of two-dimensional heterocatalysts, further promoting the ENRR field’s development.
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Tungsten
·
2025
·
IF 11.2
Qian Qi-Ling,Zeng Zhen-Yun,Chen Wan-Ting,Cheng Yu,Zhang Jia,Li Chuan-Hua,Qian Guang-Ren
The promoter is very important for effective catalysts, and the relationship among active species, promoter, and support is a hot topic in the field of catalysis. This work aims to investigate the influence of the promoter on the formation of effective active species. For this purpose, V was leached out from V-loaded TiO 2 (V/Ti) step by step, and the loaded V was classified into different species based on their performances in the catalytic oxidation of chlorobenzene. As a result, when V/Ti was co-doped with Mo or W, the chlorobenzene conversion rate was increased from 48.1% to 54.0% (Mo) or 61.0% (W) at 210 °C. The enhancement was attributed to the redistribution of V species. Specifically, 7.8% of V was “Inactive” V on V/Ti. This “Inactive” V was transformed into an “Active” species. At the same time, “Highly-active V” amounts were increased from 86.0% (V 3.3 /Ti) to 88.1% (WV 3.3 /Ti) and 87.1% (MoV 3.3 /Ti). According to the mechanism investigation, when W and Mo coexisted with V during the synthesis, V 3+ was oxidized into V 5+ , which is easily invaded into the TiO 2 , created more strong acidic sites, and activated more active lattice oxygens. These are all in favor of the effective catalytic oxidation of chlorobenzene. The new understanding of the promoter effect will help to produce a more effective catalyst using the same amount of active species. Graphical abstract
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Wei Wen,Zimei Fu,Man Zhao,Na Gao,Qinyun Yan,Liwu Qiang,Shuai He,Ze Wang,Lifang Shi,He Xiao,Jianfeng Jia
Electrocatalytic urea oxidation reaction (UOR) offers a sustainable route for wastewater remediation and energy-saving hydrogen production, yet its efficiency is hindered by the sluggish kinetics of conventional nickel-based catalysts following an indirect oxidation mechanism. Here, we report a Mo-regulated Ni 2 P-MoO x heterostructure anchored on black phosphorus (BP) nanosheets, synthesized via an innovative electrolysis-solvothermal strategy, which shifts the UOR pathway from indirect to direct oxidation. Unlike traditional NiOOH-mediated processes, which require prior Ni 2 + oxidation, the in-situ Raman and LSV results indicate that this catalyst enables urea oxidation at unprecedentedly low potentials (1.31 V vs. RHE at 10 mA cm −2 ) before Ni 2+ self-oxidation, thereby reducing the overpotential by 245 mV relative to oxygen evolution. Advanced in-situ characterizations ( In-situ FTIR, In-situ Raman , In-situ EIS) and electronic structure analyses elucidate that Mo dopants with electron-deficient 4d orbitals synergistically enhance urea adsorption via carbonyl coordination and optimize charge transfer through interfacial electronic coupling with Ni 2 P, while phosphorus modulates the d-band center. This unique configuration promotes the direct dehydrogenation of adsorbed urea by electrophilic OH species, accelerates C–N cleavage, and minimizes harmful byproducts. This Ni 2 P-MoO x /BP catalyst sustains 55 h operation at 50 mA cm −2 , demonstrating exceptional stability. This work establishes a paradigm for steering reaction mechanisms through electronic engineering, offering transformative insights for designing energy-efficient electrocatalysts for complex molecule valorization.
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高影响因子
FUEL
·
2025
·
IF 7.5
Huanhuan Gao,Daolun Liang,Yadong Sun,Jianzhong Liu
To address space constraints in solid rocket motors, this study investigates Al–Ti, Al–Zr, and Al–Mo alloys. Their high density enhances energy release per unit volume. Multidimensional analyses—thermal oxidation behavior, ignition/combustion characteristics, and agglomeration properties—were conducted to elucidate how high-density alloys influence Al-based propellant combustion performance and energy release. Results show these high-density alloys exhibit shorter ignition delay time and combustion time, effectively increasing the propellant burning rate of propellants while reducing the pressure exponent. Titration measurements reveal combustion efficiencies of 84.28% (A), 87.33% (AT), 86.79% (AZ), and 85.91% (AM). Among them, Al–Zr demonstrates the most significant optimization effect on combustion performance. Due to the low ignition threshold, Al–Ti significantly suppresses agglomerate formation and accelerates the combustion. Meanwhile, Al–Mo enhances the transport efficiency of oxidizing gases through the phase-change sublimation mechanism of MoO 3 , indirectly boosting combustion efficiency. Furthermore, this work reveals the synergistic mechanisms by which high-density alloys optimize propellant combustion performance via multiple factors. The findings confirm the technical feasibility of simultaneously achieving superior combustion performance, high energy output, and effective agglomeration suppression, providing theoretical and technological guidance for developing advanced high-energy-density solid propellants.
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