APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Shiwei Song,Yanhui Wang,Xiaoxu Liu,Xueqing Tian,Yucan Liu,Xiaodong Liu,Fanjia Sun,Yungang Yuan,Wei Li,Jianbing Zang
Seawater electrolysis achieves sustainable hydrogen production and seawater desalination in the context of the scarcity of freshwater resources, achieving two birds with one stone. In this study, we reported an Mo-doped NiFe-phosphate hollow bird-nest architecture consisting of porous nanosheets on NiFe-foam (Mo-NiFe-PO 3 /NFF) as an admired bifunctional electrocatalyst for overall seawater splitting. The introduction of Mo distorted the crystal structure of NiFe-phosphate, regulated the electronic environment around the Ni/Fe, and improved the electrocatalytic activity. Moreover, it also cooperated with phosphate polyanions to resist the Cl − from seawater and enhanced the corrosion resistance . The Mo-NiFe-PO 3 /NFF exhibited outstanding electrocatalytic performance for alkaline seawater electrolysis under a two-electrode system where only required 1.65 V voltage to drive 100 mA cm −2 . Particularly, the electrolyzer afforded industrially current density up to 500 mA cm −2 at a low voltage of 1.78 V, which were responsible for excellent durability up to 100 h. The bifunctional electrocatalyst in this study not only possessed high catalytic activity, but also effectively resisted the corrosion of Cl − in seawater.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Small
·
2026
·
IF 11.8
Hui Wang,Yanan Li,Jingjing Dou,Qing Xu,Zitong Jiang,Tao Zhang,Chaozheng He,Mingshang Jin,Xiang Li
Direct ethanol fuel cells (DEFCs) are promising clean energy devices, but their efficiency is limited by the low C-C bond cleavage efficiency of Pd-based catalysts. Herein, we synthesized In-Mo codoped Pd metallene with rich interface defects via a simple wet-chemical method, which consists of face-centered cubic, intermetallic and amorphous phases. The catalyst's structure and ethanol electrooxidation reaction (EOR) performance was systematically characterized, and the mechanism was revealed by in situ ATR-FTIR, HPLC and DFT calculations. Results showed that the optimal PdInMo metallene exhibited a C1 pathway selectivity of 73.68%, which was 12.02 time that of commercial Pd/C. Its mass activity and specific activity were 4273.8 mA mg Pd −1 and 8.36 mA cm −2 , 2.38 and 1.34 times higher than those of undoped Pd metallene (1795.9 mA mg Pd −1 and 6.25 mA cm −2 ), 6.85 and 3.83 times higher than those of commercial Pd/C (624.2 mA mg Pd −1 and 2.18 mA cm −2 ), respectively, with excellent cycling stability (75.10% activity retention). The enhanced performance was attributed to the synergistic effect of In─Mo codoping and rich interface defects: strengthened OH* adsorption, weakened CO* adsorption, and reduced C─C bond cleavage energy barrier. This study provides a novel strategy for designing high-selectivity and high-activity Pd-based catalysts for EOR.
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DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2026
·
IF 5.5
Jingqi Che,Lingying Chen,Mengran Li,Rui Shi,Jiguang Zhang,Yana Liu,Jun Wang,Yunfeng Zhu
Catalytic doping is considered one of the most efficient strategies to achieve superior performance of MgH2, as rationally designed catalytic components can exhibit synergistic effects, thereby optimizing the kinetic pathways. In this study, the hydrothermal method was adopted to prepare clustered Ni–Mo–S catalysts, which were used to modify MgH2 to enhance its kinetic performance. Experimental results demonstrate that the molar proportion of Ni to Mo significantly impacts the modification effect of Ni–Mo–S catalysts on MgH2. Furthermore, the catalyst whose molar ratio of Ni/Mo is 7:2 achieves the optimal catalytic efficiency. Specifically, at 125 °C, MgH2-5 wt % Ni–Mo–S can absorb 4.61 wt % H2 in 1200 s. At a relatively low temperature of 250 °C, it manifests a rapid dehydrogenation rate and releases 5.81 wt % H2 in 2000 s. The hydrogenation (41.98 kJ/mol) and dehydrogenation (86.41 kJ/mol) activation energies of MgH2-5 wt % Ni–Mo–S are reduced by 48.87 and 43.79% compared to as-milled MgH2, respectively. Mechanism analysis suggests that this improvement may be ascribed to the following reasons: (1) The hydrogen pump effect of Mg2Ni/Mg2NiH4 facilitates the hydrogen diffusion; (2) electron transfer between Mo species with different valence states weakens the Mg–H bonds; (3) the in situ formed MgS serves as diffusion channels for hydrogen atoms, expediting hydrogen transport. This work provides a valuable outlook for constructing highly active catalysts for MgH2 hydrogen storage.
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高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Guo Luyao,Zhuge Kaixuan,Yan Siyang,Wang Shiyi,Zhao Jia,Wang Saisai,Qiao Panzhe,Liu Jiaxu,Mou Xiaoling,Zhu Hejun,Zhao Ziang,Yan Li,Lin Ronghe,Ding Yunjie
Supported metal clusters comprising of well-tailored low-nuclearity heteroatoms have great potentials in catalysis owing to the maximized exposure of active sites and metal synergy. However, atomically precise design of these architectures is still challenging for the lack of practical approaches. Here, we report a defect-driven nanostructuring strategy through combining defect engineering of nitrogen-doped carbons and sequential metal depositions to prepare a series of Pt and Mo ensembles ranging from single atoms to sub-nanoclusters. When applied in continuous gas-phase decomposition of formic acid, the low-nuclearity ensembles with unique Pt 3 Mo 1 N 3 configuration deliver high-purity hydrogen at full conversion with unexpected high activity of 0.62 mol HCOOH mol Pt −1 s −1 and remarkable stability, significantly outperforming the previously reported catalysts. The remarkable performance is rationalized by a joint operando dual-beam Fourier transformed infrared spectroscopy and density functional theory modeling study, pointing to the Pt-Mo synergy in creating a new reaction path for consecutive HCOOH dissociations.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Jianjun Zhu,Huamei Tong,Yu Liu,Jiahui Hu,Xinyu Zheng,Mengyue Qi,Deli Jiang
Exploring integrated regulation strategies to boosting electrocatalytic performance is essential to design more efficient and inexpensive OER catalysts. Herein, amorphous and crystalline (a-c) interface engineering and heteroatom doping are integrated to construct a novel electrocatalyst containing amorphous FeSeO x and crystalline Mo-doped NiSe 2 (denoted as FeSeO x /Mo-NiSe 2 ) via pseudocrystalline replication method and selenization treatment. The resultant FeSeO x /Mo-NiSe 2 electrocatalyst with 3D hierarchical nanoarchitectures of nanorod arrays covered by interlocking nanoblocks exposes more active sites and accelerated reaction kinetics. Furthermore, a-c interface engineering and heteroatom doping can synergistically enhance the intrinsic activity and charge transfer capability of NiSe 2 by decreasing the electron diffusion distance and flexibly modulating the electronic structure, which contributes to boost the oxygen evolution reaction (OER) performance. Consequently, the obtained FeSeO x /Mo-NiSe 2 achieves a low overpotential of 205 mV at 10 mA cm −2 , which outperforms many other transitions metal selenides electrocatalysts. Density functional theory (DFT) calculations demonstrate that the formation of an internal electric field between FeSeO x and Mo-NiSe 2 accelerates charge transport and optimizes the adsorption/desorption of oxygen-containing intermediates, thereby accelerating the reaction kinetics and improving the OER performance. This work serves as a point of reference for designing innovative metal selenides based electrocatalysts combining a-c interface engineering and heteroatom doping.
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高影响因子
Carbon Energy
·
2023
·
IF 20.5
Zhichao Jia,Yang Yuan,Yanxing Zhang,Xiang Lyu,Chenhong Liu,Xiaoli Yang,Zhengyu Bai,Haijiang Wang,Lin Yang
Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions (OERs). Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will benefit their quick transition to the next catalysts. Herein, Mo-doped CoOOH was designed as a high-performance model electrocatalyst with durability for 20 h at 10 mA cm −2 . Additionally, it had an overpotential of 260 mV (glassy carbon) or 215 mV (nickel foam), which was 78 mV lower than that of IrO 2 (338 mV). In situ, Raman spectroscopy revealed the transformation process of CoOOH. Calculations using the density functional theory showed that during OER, doped Mo increased the spin-up density of states and shrank the spin-down bandgap of the 3d orbits in the reconstructed CoOOH under the electrochemical activation process, which simultaneously optimized the adsorption and electron conduction of oxygen-related intermediates on Co sites and lowered the OER overpotentials. Our research provides new insights into the methodical planning of the creation of transition-metal oxyhydroxide OER catalysts.
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高影响因子
NANOTECHNOLOGY
·
2023
·Vol. 35
·期 10
·105702
·
IF 3.5
Xuefeng Zhang,Qin Yang,Longcheng Zhang,Jun Li,Shengjun Sun,Yingchun Yang,Yuntong Sun,Xuping Sun
Seawater splitting is a compelling avenue to produce abundant hydrogen, which requires high-performance and cost-effective catalysts. Constructing bimetallic transition metal phosphides is a feasible strategy to meet the challenge. Here, an amorphous Co–Mo–P film supported on nickel foam (Co–Mo–P/NF) electrode is developed with bifunctional properties for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline seawater. Corresponding results indicate that the introduction of Mo can improve the active sites and regulate the intrinsic activity. Such a Co–Mo–P/NF behaves with prominent electrocatalytic activity towards both HER and OER, demanding low overpotentials of 193 and 352 mV at 100 mA cm‒2 in alkaline seawater, respectively. Furthermore, the assembled electrolyzer demands a pronounced overall seawater splitting activity with a low cell voltage of 1.76 V to deliver 100 mA cm−2 presenting excellent durability without obvious attenuation after 24 h continuous stability test. This work expands the horizon to develop transition metal-phosphorus electrocatalysts with robust and efficient activity for overall seawater splitting.
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PubMed
高影响因子
RARE METALS
·
2023
·Vol. 42
·期 8
·2592-2600
·
IF 8.8
Chen Jing,Chen Xuan-Le,Lu Rou,Li Yong,Pan An-Qiang
Molybdenum dioxide has aroused a wide concern as anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and high density. However, it still faces the problems of large volume changes and low electronic conductivities, which limits its practical application. Herein, necklace-like N-doped carbon nanofibers encapsulating MoO 2 nanospheres (MoO 2 @NCNFs) with Mo–C bonding have been designed to address these issues. The rational design carbon coating structure can not only enhance the electron transfer, but also markedly strengthen structural stability. As expected, the as-prepared electrode showed superior lithium storage capacity, including a high specific capacity of 1120 mAh·g −1 at 0.1 A·g −1 , and good rate performance of 502 mAh·g −1 at 4.0 A·g −1 and a prolonged cycling stability of 490 mAh·g −1 capacity retention over 3000 cycles at 4.0 A·g −1 . Graphical abstract
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高影响因子
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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高影响因子
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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高影响因子
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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高影响因子
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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