SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Heming Sun,Xiaonian Tang,Shuo Li,Ye Yao,Li Liu
The construction of the materials with one-dimensional (1D) hollow structure using Metal-organic frameworks (MOFs) as the templates has attracted much attention for applied in various fields. Herein, MOF-derived 1D Ru/Mo co-doped Co 3 O 4 hollow microtubes have been obtained via a simple solvothermal method . The as-synthesized samples are characterized by using XRD, FESEM , TEM , XPS, PL and BET. The sensing measurement reveals that when doping amount of Mo and Ru is 1% and 0.3%, the Co 3 O 4 sample exhibits the best sensing performance. Specially, 0.3% Ru/Mo-Co 3 O 4 sample exhibits high responses of 126–100 ppm TEA at a low operating temperature of 160 °C, which are about 18.5 times than that of pure Co 3 O 4 . Furthermore, it shows rapid response/ recovery speed (5 s/7 s), good selectivity and repeatability as well as excellent long-term stability. The good TEA sensing performance is attributed to the construction of 1D hollow architecture and synergistic effect of Ru/Mo co-doping. Thus, it is expected to be a promising sensing material for high-performance detection of TEA gas. In addition, this work provides an useful inspiration for preparation of MOF-derived materials with 1D hollow architecture for achieving excellent performance in various fields.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xinyang Dong,Yundong Cao,Jiayuan Zhang,Linlin Fan,Mingliang Wang,Hong Liu,Guanggang Gao
Lithium-sulfur batteries (LSBs) present wide range of market and tremendous application potential. Nevertheless, the “shuttle effect” of lithium polysulfides (LiPSs) and the sluggish redox kinetics restrict their large-scale application. We report herein the Mo-substituted Keggin type H 3 PW 10 Mo 2 O 40 (PW 10 Mo 2 ) evenly decorated on the MWCNTs conductive framework by electrostatic attraction as the functional interlayer materials. W and Mo atoms in PW 10 Mo 2 provide chemical adsorption sites for polysulfides, and density functional theory (DFT) calculations further confirm that Mo sites possess stronger capture ability to LiPSs than that of W sites. Meanwhile, the Mo implantation can effectively expedite the redox reaction of LiPSs. Furthermore, MWCNTs afford the plentiful attachment points for PW 10 Mo 2 , thus exposing abundant active sites to adsorb and catalyze polysulfides. The resulting cells demonstrate superior discharge capacity of 1064.9 mAh g −1 under 0.2C up to 100 cycles as well as excellent long-life cycling stability with low recession rate of 0.051 % under 3C up to 1000 cycles. Our work illustrates the effect of Mo atom substitution of polyoxotungstates as interlayer materials and thereby provides a new strategy for developing LSBs with superior reversible capacity and long cycling performance.
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ChemElectroChem
·
2023
·Vol. 10
·期 3
·e202201087
·
IF 4
Shaojie Gao,Ping Li,Yao Shi,Yi He,Lecheng Lei,Shaoyun Hao,Xingwang Zhang
Graphical Better with defects : A ternary alloy PtCoMo nanocatalyst with dual surface Co and Mo vacancy defects was used as an efficient electrocatalyst for acidic oxygen reduction reaction for fuel cell applications. Proton exchange membrane fuel cell (PEMFC) is considered as the most promising energy conversion technology, which is hampered by the unsatisfied activity and high loading of Pt. The performance of Pt-based catalyst toward PEMFC depends on the surface bond length of Pt−Pt, which is closely related to the surface defect engineering. Here we firstly present a ternary alloy PtCoMo nanocatalyst with dual surface Co and Mo vacancy defects (V Co−Mo −PtCoMo) that compressed the Pt−Pt bonds, thus exhibiting an outstanding activity toward oxygen reduction reaction (ORR) with a mass activity of 0.57 A mg Pt −1 at 0.9 V (RHE, reversible hydrogen electrode), which is 5.2 times higher as compared with commercial Pt/C (20 wt %) in 0.1 M HClO 4 . The characterizations and density functional theory calculations demonstrate that the Pt−Pt bonds are significantly compressed through the dual surface defects, thus weakening the binding energy and effectively enhancing the acidic ORR performance.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 6
·2780-2786
·
IF 10.733
Zhen Zhang,Ping Li,Qi Wang,Qi Feng,Youkun Tao,Jiaoyan Xu,Cheng Jiang,Xiner Lu,Jiantao Fan,Meng Gu,Hui Li,Haijiang Wang
As a cheaper Pt-group metal, ruthenium (Ru) is a highly competitive alternative to Pt for commercialization towards the hydrogen evolution reaction (HER). Herein, we report the modulation effect on the Gibbs free energy (ΔGH*) of hexagonal-close-packed (hcp) Ru resulting from heteroatom Mo doping. In particular, for the first time the hcp MoRu3 crystal structure is theoretically predicted with pretty high intrinsic HER activity. Meanwhile, the Mo hetero-dopant could act as a new active site with Pt-like ΔGH*. Motivated by the prediction, we report a novel metal organic framework (MOF)-assisted synthetic strategy to prepare a Mo-doped hcp Ru electrocatalyst. Accordingly, the hcp MoRu3 catalyst exhibits an ultralow overpotential of 30.5 mV at 10 mA cm−2, ensuring excellent Pt-like intrinsic HER activity. More importantly, the excellent electrochemical performance measured with a proton exchange membrane (PEM) electrolyzer further highlights the promising potential of the hcp MoRu3 catalyst for hydrogen production.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Ruiyang Zhang,Penghui Li,Fang Wang,Liqun Ye,Abhijeet Gaur,Zeai Huang,Ziyan Zhao,Yang Bai,Ying Zhou
Atomically dispersed atom catalysts with atomically distributed active metal centers have attracted great attention owing to the maximum atom efficiency and excellent selectivity. Herein, for the first time, we found atomically dispersed Mo atoms can be formed on g-C 3 N 4 , and induce its amorphous transformation. This amorphous transformation leads to the formation of strong band tails with remarkably enhancing the absorbance edge of Mo-C 3 N 4 up to 750 nm, resulting in almost whole visible-light range absorption. The formation of new Mo-C and Mo-N bonds due to strong interfacial interaction between atomically dispersed Mo atoms and g-C 3 N 4 provide new electron and hole transport pathways to accelerate the separation of charge carriers. As a result, amorphous Mo/C 3 N 4 (a-Mo/C 3 N 4 ) reveals excellent photoreduction of CO 2 , yielding CO and H 2 productions of 18 and 37 μmol g −1 h −1 under visible-light illumination (λ > 420 nm), which manifest a remarkable 10.6- and 4-folds enhancement of that over crystalline g-C 3 N 4 . This finding provides a conceptually different approach to fabricate high-efficient photocatalyst through the strong interfacial interaction between atomically dispersed metal atoms and host.
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Small
·
2018
·Vol. 14
·期 27
·1800090
·
IF 9.598
Lianshan Sun,Chunli Wang,Xuxu Wang,Limin Wang
Controllable synthesis of functional materials is of widespread interest for particle engineering. Such a method has not been widely promoted due to the lack of recognition of the fundamental principle, especially for organic–inorganic hybrid materials. Here, as an entrance, the controllable synthesis of Mo-polydopamine coordination flowers is realized through a facile foaming method, and a 2D nanopetal as the building monomer of the flower is synthesized. Depending on the morphology evolution of Mo-dopamine complex under different conditions, and the surface iterative topology growth of the Mo-polydopamine petal, the reasons of why the Mo-polydopamine complex self-assembles into a flower structure can be attributed to the synergistic effect of multicore symbiosis and structural self-protective growth behaviors. Benefiting from the strong structure stability of the Mo-polydopamine nanopetal, a hybrid structure of MoO 2 quantum dot in situ anchoring in the N-doped 2D carbon framework is prepared by direct pyrolysis, which shows a highly reversible performance in application for lithium-ion secondary batteries (LIBs). This work enhances the possibility for the controllable synthesis of organic–inorganic hybrid materials by adjusting the multicore intergrowth and inhibiting the interfacial assembly.
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高影响因子
TRANSACTIONS OF TIANJIN UNIVERSITY
·
2018
·Vol. 25
·期 1
·52-65
·
IF 0
Li Wang,Zhang Qingjun,Zeng Aiwu
In this study, liquid-phase aerobic oxidation of toluene catalyzed by Mn–Mo oxide was conducted in a 1.0 L batch reactor. The macroscopic kinetics of toluene consumption and benzaldehyde generation at 413–443 K were obtained from a combination of experimental observation and hypothetical models. The results clearly showed that both the oxidation rate of toluene and generation rate of the aromatic product were proportional to the concentration of the substrate, the partial pressure of oxygen and the surface area of the catalyst. The energy barrier of toluene oxidation to benzyl alcohol was the highest (≈ 81 kJ mol −1 ), while that of benzyl alcohol oxidation to benzaldehyde was the lowest (≈ 57 kJ mol −1 ). Moreover, the activation energy of further oxidation of benzaldehyde in an acetic acid solvent was only slightly lower (≈ 1.9 kJ mol −1 ) than that of toluene oxidation. Significantly, the transformation of benzyl alcohol indeed contributed to the generation of benzaldehyde and this step conformed to a first-order parallel-consecutive model. Increased reaction temperature and residence time favored the transformation of benzyl alcohol to benzaldehyde. In addition, doping with molybdenum at Mn/Mo = 3/1 enhanced the catalytic performance of the heterogeneous catalyst and was attributed to the presence of a synergetic effect between different metal cations. Regarding the microscopic kinetics, the LH-OS-ND mechanism (Langmuir–Hinshelwood adsorption of reagents on the same type of active sites and non-dissociative adsorption of oxygen) was verified as responsible for the heterogeneous oxidation of toluene. Oxygen and benzaldehyde were weakly adsorbed (Δ H ads,Oxy ≈ − 15 kJ mol −1 , Δ H ads,Bald ≈ − 30 kJ mol −1 ), but showed strong mobility (Δ S ads,Oxy ≈ − 22 J mol −1 K −1 ), Δ S ads,Bald ≈ − 39 J mol −1 K −1 ). The fundamental intrinsic rates were deduced based on the LH-OS-ND mechanism and showed great consistency with the macroscopic results.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 19
·9228-9235
·
IF 9.931
Teng Wang,Rumei Jin,Xiuqi Wu,Jie Zheng,Xingguo Li,Kostya Ostrikov
A highly efficient Ni–Mo bimetallic catalyst for the hydrogen evolution reaction can be obtained from a molybdate incorporated Ni-MOF by thermal decomposition in NH3. The catalyst is composed of crystalline Ni nanoparticles doped with amorphous low valence Mo oxide encapsulated in thin N-doped carbon layers, showing excellent HER performance, featuring a very low overpotential for the HER (η20 = 58 mV), low Tafel slope (57 mV dec−1) and excellent long term stability. The catalyst apparently outperforms N-doped carbon encapsulated Ni catalysts without Mo doping, emphasizing the critical synergetic effect of Mo doping and the surface N-doped carbon thin layer on promoting the performance of Ni based HER catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Wenhao Zhang,Yuanhao Tang,Liangmin Yu,Xin-Yao Yu
Nickel-based metal oxides/hydroxides are promising electrocatalysts for oxygen evolution reaction. However, their electrocatalytic activity for hydrogen evolution reaction (HER) is very poor. Herein, taking Mo-incorporated nickel hydroxide (Mo-Ni(OH) 2 ) as an example, a facile, time-efficient, and low-temperature H 2 /N 2 plasma activation strategy is developed to activate the HER performance by constructing heterostructure. This kind of heterostructure is composed of metal, metal alloy, metal nitride , and oxygen vacancy-riched metal hydroxide with more exposed catalytically active sites, enhanced mass activity, and accelerated electron transport. The optimized plasma-activated Mo-Ni(OH) 2 (P-Mo-Ni(OH) 2 ) manifests superior HER performance to pristine Mo-Ni(OH) 2 and even comparable to the benchmark Pt/C catalyst in alkaline solution. Moreover, when assembling a two-electrode urea-assisted water electrolysis system by using P-Mo-Ni(OH) 2 as both cathode and anode, the assembled cell only need a small voltage of 1.36 V to achieve a current density of 10 mA cm −2 and exhibits extremely stable catalytic performance up to 1000 h.
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Small
·
2017
·Vol. 13
·期 41
·1701648
·
IF 8.643
Qian Zhang,Pengsong Li,Daojin Zhou,Zheng Chang,Yun Kuang,Xiaoming Sun
Hydrogen evolution reaction (HER) has prospect to becoming clean and renewable technology for hydrogen production and Ni–Mo alloy is among the best HER catalysts in alkaline electrolytes. Here, an in situ topotactic reduction method to synthesize ultrathin 2D Ni–Mo alloy nanosheets for electrocatalytic hydrogen evolution is reported. Due to its ultrathin structure and tailored composition, the as-synthesized Ni–Mo alloy shows an overpotential of 35 mV to reach a current density of 10 mA cm −2 , along with a Tafel slope of 45 mV decade −1 , demonstrating a comparable intrinsic activity to state-of-art commercial Pt/C catalyst. Besides, the vertically aligned assemble structure of the 2D NiMo nanosheets on conductive substrate makes the electrode “superaerophobic,” thus leading to much faster bubble releasing during HER process and therefore shows faster mass transfer behavior at high current density as compared with drop drying Pt/C catalyst on the same substrate. Such in situ topotactic conversion finds a way to design and fabricate low-cost, earth-abundant non-noble metal based ultrathin 2D nanostructures for electrocatalytic issues.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xilin Wu,Shun-Xing Liang,Lingjie Jia,Yufeng Liu,Yuexian Huang,Yujing Liu,Liang-Yu Chen,Yuanzheng Yang,Pingjun Tao
The inherent limitations of conventional metallic glass (MG) catalysts in adapting to complex water environments over a wide pH range stem from their monotonic active site, which is incapable of simultaneously fulfilling multiple functional purposes. Herein, we overcome the narrow range of pH adaptability of existing advanced oxidation catalysts by designing a series of quinary FeCoNiMoB medium-entropy alloys in amorphous structure (referred to as A-MEAs). In particular, the slight modulation of Mo to obtain Fe 25 Co 25 Ni 25 Mo 0.5 B 24.5 A-MEA with highest Gibbs free energy achieves a complete degradation of pollutants both at acidic and alkaline conditions in 10 min. This performance surpasses that of most traditional MGs and high-entropy alloys (HEAs) constrained by the composition limits for entropy maximization. Further insights reveal that in both cases, the multi-site synergistic effects of Mo-driven fast electron transfer of M (M = Fe, Co, and Ni) as active sites and surface-mediated reaction cycles of M 2 + /M 3+ contribute to the accelerated transformation of reactive oxygen species (ROS) from peroxydisulfate (PDS) and the remarkable catalytic performance of A-MEAs. The radical evolution demonstrates that SO 4 ·‾ plays a major role under acidic conditions while O 2 ·‾ dominates the catalytic reactions under alkaline conditions. Accordingly, this work aims to fill the gap of A-MEAs for catalytic oxidation of organic pollutants and provide the design strategy of novel MEA catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiabing Luo,Yongxiao Tuo,Jianchao Zhang,Wenle Li,Shutao Wang,Yanpeng Li,Yuan Pan,Yan Zhou,Jun Zhang
The development of efficient and low-cost overall water splitting electrocatalysts for an anion exchange membrane (AEM) electrolyzer is desirable for hydrogen production. The control of geometric and electronic structures of electrocatalysts can improve the catalytic efficiency of hydrogen evolution reaction (HER) and durability in oxygen evolution reaction (OER). Spatially confined growth and heteroatom doping can achieve this prospect of the target electrocatalysts. Herein, we prepared a carbon-shell confined Mo-doped CoP electrocatalyst (Mo-CoP@C) via an anion adsorption coupled pyrolytic phosphorization method. A Metal-Organic Framework (MOF) of Co was used to achieve Mo doping and carbon-shell encapsulation. Mo doping significantly altered the electronic structure of CoP, which produced a local polarized environment for water dissociation during alkali HER process. Meanwhile, carbon-shell confined growth and provided a protective layer for durable OER process. Consequently, Mo-CoP@C exhibits attractive alkali electrocatalytic HER and OER activities with the overpotentials of 122 and 280 mV at 0.01 A cm −2 . Finally, the assembled Mo-CoP@C-CP‖Mo-CoP@C-TFF AEM electrolyzer could operate for 500 h at 0.1 A cm −2 .
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