COMPOSITES PART B-ENGINEERING
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2025
·
IF 14.2
Bingbing Qiu,Donghui Zhang,Ruiming Fang,Yanfang Wang,Banglong Shen,Junhao Dai,Huaqiang Chu
Electrocatalytic hydrogen production is a green and feasible method for obtaining hydrogen energy. However, the bottlenecks of high cost, low catalytic activity and inferior stability urgently need to be addressed, and constructing advanced catalysts with optimized microscopic morphology and crystal structure is a feasible and effective strategy to overcome this barrier. Herein, an artful strategy of in-situ grown coupled with N doping and C encapsulation was employed to obtain the NC/NiO–Mo/NF with biomimetic cattle stomach-liked porous structure, which can offer shortcut for ion transportation and expose more active sites for H∗ adsorption. Particularly, the constructed NiMoO 4 –NiO heterojunction in NC/NiO–Mo/NF can significantly boost the hydrogen evolution activity. Meanwhile, the density functional theory (DFT) confirm that the construction of the crystalline-amorphous heterojunction induces electron transfer from NiMoO 4 to NiO, promoting a downshift in the d-band center, thereby achieving a near-thermoneutral free energy for the hydrogen evolution reaction (HER). The de-signed electrocatalyst exhibits exceptional HER activity, with a small overpotential of 48 mV to achieve a current density of 10 mA cm −2 . It is important that NC/NiO–Mo/NF exhibits exceptional HER stability, with current density of 50 mA cm −2 for 100 h. The finding provides a feasible strategy for the fabrication of nonprecious-metal-based HER electrocatalysts with high activity and stability toward industrial water electrolysis.
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JOURNAL OF ALLOYS AND COMPOUNDS
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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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Journal of the American Chemical Society
·
2024
·
IF 14.4
Yanliang Zhou,Lili Liang,Congying Wang,Fuxiang Sun,Lirong Zheng,Haifeng Qi,Bin Wang,Xiuyun Wang,Chak-tong Au,Junjie Wang,Lilong Jiang,Hideo Hosono
To date, NH3 synthesis under mild conditions is largely confined to precious Ru catalysts, while nonprecious metal (NPM) catalysts are confronted with the challenge of low catalytic activity due to the inverse relationship between the N2 dissociation barrier and NHx (x = 1–3) desorption energy. Herein, we demonstrate NPM (Co, Ni, and Re)-mediated Mo2CTx MXene (where Tx denotes the OH group) to achieve efficient NH3 synthesis under mild conditions. In particular, the NH3 synthesis rate over Re/Mo2CTx and Ni/Mo2CTx can reach 22.4 and 21.5 mmol g–1 h–1 at 400 °C and 1 MPa, respectively, higher than that of NPM-based catalysts and Cs–Ru/MgO ever reported. Experimental and theoretical studies reveal that Mo4+ over Mo2CTx has a strong ability for N2 activation; thus, the rate-determining step is shifted from conventional N2 dissociation to NH2* formation. NPM is mainly responsible for H2 activation, and the high reactivity of spillover hydrogen and electron transfer from NPM to the N-rich Mo2CTx surface can efficiently facilitate nitrogen hydrogenation and the subsequent desorption of NH3. With the synergistic effect of the dual active sites bridged by H-spillover, the NPM-mediated Mo2CTx catalysts circumvent the major obstacle, making NH3 synthesis under mild conditions efficient.
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Yijie Wang,Xudong Wu,Dan Chen,Linqian Hou,Dezhi Yang,Hong Li,Yaling Yang
The rapid and sensitive detection of glyphosate herbicide in agricultural products is urgent need. Herein, we develop a photosensitive Fe 3 O v -Mo/P nanozyme with defect-rich rough surface by the co-precipitation method. In particular, the Fe 3 O v -Mo/P nanozyme with high-percentage oxygen vacancy (OV) defects and rough surface exhibited superior peroxidase (POD)-like activity and kinetics. More intriguingly, Fe 3 O v -Mo/P nanozyme with strong optical absorption in near-infrared (NIR) region showed excellent light-promoted POD-like activity. It was found that the defect-rich rough surface is conducive to the adsorption of glyphosate to inhibit the POD-like activity of Fe 3 O v -Mo/P. Under near-infrared laser irradiation, the inhibitory effect of glyphosate on the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) by Fe 3 O v -Mo/P was increased by 2.64 times. A colorimetric platform was developed for the detection of glyphosate with a low detection limit of 0.032 mg L -1 and good selectivity. The method was used to determine the residual glyphosate in coffee, and the recovery efficiency was between 91.20–104.00 %. This work that combines the advantage of defect engineering and NIR provides a strategy for developing high-active nanozyme in pesticide assay.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xiaonan Xu,Nana Luo,Wan-Hui Wang,Ming Bao,Jiasheng Wang
Fatty acid hydrogenation is an important method for the production of fatty alcohols. The combination of Ni and Mo has been reported to be an effective and low-cost catalyst. However, the effect of Mo doping has yet to be fully understood. Here Ni-MoOx/TiO2 catalysts were prepared via simple impregnation. and the enhancement effects of Mo doping were comprehensively revealed. First, MoOx can attract electrons from Ni, reduce the electron density of Ni to improve the intrinsic activity of Ni, and form a Niδ+-(MoOx)δ− heterojunction to induce H2 heterolytic cleavage to active hydrogen ions. Second, the reduction of MoOx generates oxygen vacancies, which can absorb C═O of the fatty acid and facilitate the reaction progression. Third, a Ni1–xMox solid solution can be formed, which can increase the hydrogen adsorption quantity and accelerate the reaction rate. Finally, the bond strength of Mo–O is found to be the most optimum that can absorb the fatty acids while releasing the alcohols so as to recover the oxygen vacancies and avoid overhydrogenation. Therefore, high activity and selectivity for the hydrogenation of carboxylic acid substrates to alcohols can be obtained. Under significantly milder conditions (155 °C, 3 MPa H2) the catalyst provided a 98% yield of lauryl alcohol from lauric acid hydrogenation with a low activation energy of 40.1 kJ/mol. This work could provide an insightful understanding about the effects of Mo doping to Ni on catalyzing hydrogenation reactions.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Yu-Zhen Xu,Yu-Le Wang,Yu-Dong Shan,Song-Hai Wu,Yong Liu,Xu Han
Selective oxidation of cyclohexene (Cy) to cyclohexene oxide (Cy-ep) by O2 under solvent- and initiator-free conditions is a challenge in chemical processes, which is still constrained by its low selectivity (theoretical selectivity of 50.0%). Given the low epoxide selectivity (<20.0%) of single metal catalysts, we propose a relay catalysis strategy on the oxidation of Cy to Cy-ep with high selectivity by the spherical Mg–Mo bimetallic oxide (MMO). Such a relay catalyst exhibits a desirable Cy conversion of 31.0% and a high selectivity of 49.3% toward Cy-ep. Meanwhile, the high stability and reusability of MMO also indicate its potential to be used for industrial scale-ups. A series of characterizations and DFT calculations reveal that the negatively charged lattice oxygen in [MgII–O–II] adsorbs allylic H of Cy to weaken the bond energy of the allylic C–H bond and form Cy•, and then Cy• rapidly traps O2 to give CyOO•, which subsequently abstracts H from allylic C–H of another Cy to form 2-cyclohexene-1-hydroperoxide (Cy-OOH) and Cy•, achieving the propagation cycle. On the other hand, the Mo(VI) site in MMO catalyzes the produced Cy-OOH peroxo, which then oxidizes Cy to Cy-ep and 2-cyclohexene-1-ol. This work provides insight into the relay catalyst for the epoxidation of olefin with O2 with high selectivity under solvent- and initiator-free conditions.
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Yi Li,Shan Yu,Yuehan Cao,Yue Huang,Qiaohao Wang,Yuangang Duan,Lina Li,Kaibo Zheng,Ying Zhou
Maximizing ultrafast electron-transfer kinetics in semiconductor is pivotal but challenging for high-efficiency solar-to-energy during the photocatalytic reaction process due to the intrinsic property of photocatalysts with low surface electron density. Herein, a model photocatalyst CdS@Mo is synthesized through a typical hydrothermal method for modulating the ultrafast electron-transfer to enhance the surface electron density. X-ray absorption fine spectra (XAFS) reveal that Mo is coordinated with S atoms to form a Mo-S 6 configuration which is different from common MoS 2 and Mo foil structures. Based on the femtosecond transient absorption spectra (fs-TAS), it is found that the formation of Mo-S 6 configuration contributes to the fast decay of CdS signal and Mo-S 6 signal reactivation, illustrating the ultrafast electron-transfer (∼2.2 ps) from CdS to Mo-S 6 configuration, which achieves the enhanced electron density of photocatalyst surface. Finally, a holistic photocatalytic performance evaluation discloses that the growing of Mo-S 6 configuration obviously improves the photocatalytic hydrogen evolution (PHE) efficiency of CdS from 28.5 to 47.5 mmol g –1 h –1 with a solar-to-hydrogen (STH) efficiency of 0.10 % which is seldomly discussed in the system containing sacrificial agents. This work opens a new path to modulate the surface electron density by tuning the ultrafast electron-transfer for enhancing reaction efficiency in electron-density-dependent systems.
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SENSORS
·
2025
·Vol. 25
·期 9
·2634
·
IF 3.5
Mengxue Xu,Yihong Zhong,Hongpeng Zhang,Yi Tao,Qingqing Shen,Shumin Zhang,Pingping Zhang,Xiaochun Hu,Xingqi Liu,Xuhui Sun,Zhenxing Cheng
HighlightsWhat are the main findings?The problem of dichloromethane “poisoned” MOS materials was well solved.Gas sensing mechanism of dichloromethane on the MOS material was elucidate.What is the implication of the main finding?The best performance of significant response and excellent recoverability by the MEMS sensor to dichloromethane is attributed to a synergetic effect from Mo and Ni co-doping into SnO2.Kinetically, the transportation of dichloromethane molecules onto the surface determines the response process. Thermodynamically, the output steady electronic signal of the MEMS sensor follows the equations newly derived by statistical mechanics.The challenging problem of chlorine “poisoning” SnO2for poorly recoverable detection of dichloromethane has been solved in this work. The materials synthesized by Ni or/and Mo doping SnO2were spread onto the micro-hotplates (<1 mm3) to fabricate the MEMS sensors with a low power consumption (<45 mW). The sensor based on Mo·Ni co-doped SnO2is evidenced to have the best sensing performance of significant response and recoverability to dichloromethane between 0.07 and 100 ppm at the optimized temperature of 310 °C, in comparison with other sensors in this work and the literature. It can be attributed to a synergetic effect of Mo·Ni co-doping into SnO2as being supported by characterization of geometrical and electronic structures. The sensing mechanism of dichloromethane on the material is investigated. In situ infrared spectroscopy (IR) peaks identify that the corresponding adsorbed species are too strong to desorb, although it has demonstrated a good recoverability of the material. A probable reason is the formation rates of the strongly adsorbed species are much slower than those of the weakly adsorbed species, which are difficult to form significant IR peaks but easy to desorb, thus enabling the material to recover. Theoretical analysis suggests that the response process is kinetically determined by molecular transport onto the surface due to the free convection from the concentration gradient during the redox reaction, and the output steady voltage thermodynamically follows the equation only formally identical to the Langmuir–Freundlich equation for physisorption but is newly derived from statistical mechanics.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Junshuo Cui,Shuang Liu,Liangyu Guo,Zhongjun Li,Zuozhen Zhang,Ying Xiong
Uniform dispersion of graphene is a prerequisite for the preparation of high-performance graphene-based composites. In this study, a new type of coupling agent which contains a thiophene center and two silanol groups (TPSi) is synthesized via amino-epoxy ring-opening reaction. The molecule shows good ability for dispersing graphene in water based on its amphiphilic feature. Dynamic light scattering (DLS) reveals that the concentration of graphene reaches 3 mg mL −1 at the weight ratio of TPSi-to-graphene of 1:1. It also stabilizes graphene well when diminishing the weight ratio to 0.5:1. By freeze-drying the dispersion, TPSi/graphene composite is prepared and it shows good adsorption performance for Mo(VI) in water. The maximum capacity can reach to 134.87 mg g −1 at pH 3 according to the Langmuir isotherm model. The composite also exhibits fast adsorption kinetics that equilibrium could be achieved within 2 h. TPSi plays a key role for the uniform distribution of graphene and improves the adsorption capability of graphene-based composite for Mo(VI) ions.
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Desalination and Water Treatment
·
2025
·
IF 1
Qian Wang,Haifeng Yang,Shanni Lin,Wei Ji,Shu Zhang,Wenjie Wang,Jiazheng Yu,Jingwen Gao,Xiulei Fan
The advanced oxidation processes (AOPs) employing bimetallic catalysts for peroxodisulfate (PDS) activation has attracted considerable attention. A novel composite, polyethylene mulch-sorghum straw biochar (Fe-Mo 0.1 /N-PSC), was synthesized via hydrothermal activation, co-impregnation, and high-temperature pyrolysis to enhance catalytic efficiency and facilitate agricultural solid waste valorization. In the Fe-Mo 0.1 /N-PSC/PDS system, this composite efficiently activated PDS, achieving 91.86 % tetracycline (TC) removal within 3 minutes, with a pseudo-first-order rate constant of 0.1426 min⁻¹ , surpassing comparable catalytic systems. The influences of PDS concentration, catalyst dosage, pH, and temperature on TC degradation were systematically investigated. X-ray photoelectron spectroscopy indicated that the reactive Mo 4 + promoted the cycle of Fe²⁺/Fe³ ⁺, accelerating reaction kinetics. Quenching and electron paramagnetic resonance analyses confirmed the generation of radicals (•OH, SO₄•⁻, O₂•⁻), which actively contributed to TC degradation. Additionally, the persistent free radicals derived from PE during hydrothermal activation further enhanced degradation efficiency. Liquid chromatography-mass spectrometry identified degradation intermediates, elucidating possible pathways and proving the toxicity of intermediates greatly reduced. The system exhibited excellent stability, maintaining over 75 % degradation efficiency after five cycles with minimal metal leaching, offering valuable insights for practical applications. This study highlights Fe-Mo 0.1 /N-PSC as an effective PDS catalyst and a sustainable strategy for agricultural waste reutilization.
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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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高影响因子
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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