ADVANCED FUNCTIONAL MATERIALS
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2024
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IF 18.5
Juncong Zou,Xiang Li,Shanying He,Qiuya Niu,Shaohua Wu,Chunping Yang
Heterogeneous interfaces designed rationally in catalysts can induce geometrical, compositional, and electronic effects that can be applied to modulate catalytically active sites and consequently accelerate reaction kinetics. Here, a core-shell heterostructure catalyst consisting of crystalline molybdenum phosphide (MoP) cores and amorphous tungsten oxide (WO x ) shells on porous carbon nanosheets (PCN) is developed for oxidative desulfurization (ODS) of fuels. The strongly coupled core-shell heterogeneous interface triggers a distinctive atomic permeation effect that induces substantial electron transfer from MoP to WO x and subsequent generation of electron-rich W sites, consequently optimizing the adsorption of intermediates and substrates. The resulting catalyst (WO x @MoP/PCN) demonstrates a turnover frequency as high as 768.1 h −1 for ODS at 60 °C, exceeding that of almost all the state-of-the-art ODS catalysts by 1–2 orders of magnitude. Moreover, a novel surface oxidation pathway based on direct electron transfer is identified in the WO x @MoP/PCN-H 2 O 2 system, which bypasses the formation of reactive oxygen species, consequently endowing the system with a moderate redox potential. Thus, WO x @MoP/PCN exhibits unprecedented selectivity, achieving 100% removal of thiophenic sulfides from real diesel with minimal consumption of oxidant.
研究领域:
催化化学
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能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2021
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IF 6.901
He-Qiang Chang,Guo-Hua Zhang,Kuo-Chih Chou
Electrochemical water splitting is considered a sustainable route for the hydrogen industry. In this work, Mo 2 C/MoC heterostructure supported on N -doped carbon (Mo 2 C/MoC@NC) was prepared via a carbonization strategy. For the product (Mo 2 C/MoC@NC-1-2) fabricated with a g-C 3 N 4 / ammonium molybdate tetrahydrate molar ratio of 1:2 at 700 °C under 10%CH 4 /H 2 atmosphere, a high stability and good HER activity with a η 10 of 113 mV in 1M KOH were achieved. To further enhance the catalytic performance of the synthesized Mo 2 C/MoC@NC, the phosphating strategy was proposed for the preparation of Mo 2 C/MoC/MoP heterostructure supported on N-doped carbon (Mo 2 C/MoC/MoP@NC). When the precursor Mo 2 C/MoC@NC-1-2 was phosphated at 650 °C with a heating rate of 5 °C min −1 and kept for 0 min, the as-synthesized Mo 2 C/MoC/MoP@NC-650-0 exhibits good HER catalytic activity with a pretty low η 10 of 78 mV, a j 0 of 0.398 mA cm −2 , and a Tafel slope of 52 mV dec −1 in 1M KOH. This good activity of HER can be ascribed to the N-doped carbon as substrate and the construction of transition metal-based heterostructures.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
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2023
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IF 11.9
Luyao Zheng,Cong Liu,Wenbiao Zhang,Boxu Gao,Tianlan Yan,Yahong Zhang,Xiaoming Cao,Qingsheng Gao,Yi Tang
To design and build effective electrocatalysts for water splitting is a key challenge, but hardly any non-noble metal catalysts can match the performance of Pt at cathodes and Ir or Ru at anodes. The synergistic combination of non-noble metal catalysts could be a better option for overall water splitting (OWS). Herein, a heterostructured electrocatalyst of MoP/CoMoP2 nanoparticles embedded in N, P-doped carbon matrix (MoP/CoMoP2@NPC) was fabricated via reticular chemistry. Results indicate that, due to the cooperative effect of MoP/CoMoP2 interfaces and phosphorous vacancies, MoP/CoMoP2@NPC shows the extraordinarily efficiency and robust stability for hydrogen/oxygen evolution reactions and OWS in a wide pH range. This work could offer a promising interface-engineering approach to develop and build effective cooperative electrocatalysts for the sustainable production of hydrogen.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Dongfeng Sun,Songmin Lin,Yuan Yu,Shengwei Liu,Fangyou Meng,Gaohui Du,Bingshe Xu
Transition metal phosphides are novel electrocatalysts that can be used to replace noble metals for the electrochemical production of hydrogen. In this work, N and P co-doped carbon-coated cobalt-doped molybdenum phosphide (CoMoP@N,P-C) nanoparticles are explored as electrocatalyst for overall water splitting. The presence of a unique three-dimensional (3D) porous structure in CoMoP@N,P-C offers abundant catalytic active sites for the penetration of the electrolyte solution, thereby facilitating the transfer of ions. In addition, cobalt doped into MoP increases the catalytic activity, and N and P co-doped carbon improves the electrical conductivity of the carbon matrix. Subsequently, the synergy between CoMoP cores and N, P-C shells enhances the total hydrolysis performance of the electrocatalyst in hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) processes. At a current density of 10 mA/cm 2 in 1 M KOH, HER and OER overpotential of the CoMoP@N, P-C are 152 mV and 296 mV, respectively. Moreover, the cell voltage of CoMoP@N, P-C as a bifunctional electrode for overall water splitting is 1.62 V (at 10 mA/cm 2 ), which is close to that of the full noble-metal electrode (RuO 2 || Pt/C, 1.58 V). Overall, the CoMoP@N, P-C bifunctional catalyst shows great potential for replacing noble-metal electrodes in water splitting applications.
研究领域:
材料科学
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电化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
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2021
·Vol. 50
·期 13
·4555-4566
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IF 4.39
Ishaq Muhammad,Maher Jabeen,Peiran Wang,Yu-Shi He,Xiao-Zhen Liao,Zi-Feng Ma
The advancement of novel synthetic approaches for micro/nanostructural manipulation of transition metal phosphide (TMP) materials with precisely controlled engineering is crucial to realize their practical use in batteries. Here, we develop a novel spray-drying strategy to construct three-dimensional (3D) N,P co-doped graphene (G-NP) microspheres embedded with core–shell CoP@C and MoP@C nanoparticles (CoP@C⊂G-NP, MoP@⊂G-NP). This intentional design shows a close correlation between the microstructural G-NP and chemistry of the core–shell CoP@C/MoP@C nanoparticle system that contributes towards their anode performance in lithium-ion batteries (LIBs). The obtained structure features a conformal porous G-NP framework prepared via the co-doping of heteroatoms (N,P) that features a 3D conductive highway that allows rapid ion and electron passage and maintains the overall structural integrity of the material. The interior carbon shell can efficiently restrain volume evolution and prevent CoP/MoP nanoparticle aggregation, providing excellent mechanical stability. As a result, the CoP@C⊂G-NP and MoP@⊂G-NP composites deliver high specific capacities of 823.6 and 602.9 mA h g−1 at a current density of 0.1 A g−1 and exhibit excellent cycling stabilities of 438 and 301 mA h g−1 after 500 and 800 cycles at 1 A g−1. The present work details a novel approach to fabricate core–shell TMPs@C⊂G-NP-based electrode materials for use in next-generation LIBs and can be expanded to other potential energy storage applications.
研究领域:
材料科学
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能源存储
✓ 已验证
DOI
PubMed
高影响因子
CRYSTAL GROWTH & DESIGN
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2021
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IF 4.076
Di Wu,Bei Zhang,Qichao Yao,Baohong Hou,Lina Zhou,Chuang Xie,Junbo Gong,HongXun Hao,Wei Chen
Screening of suitable coformers is a major challenge during the development of cocrystals. To guide and simplify the cocrystal synthesis process, we evaluated three different predictive methods as well as their combinations during the cocrystallization of 2-amino-4,6-dimethoxypyrimidine (MOP) with 63 components. The conductor-like screening model for the real solvents (COSMO-RS) approach offered the best predictive results among three methods with an overall success rate of 84.1%. When combined with molecular complementarity (MC) analysis, the success rate was up to 85.7%. The Hansen solubility parameters (HSP) method did not deliver a satisfying outcome no matter if used individually or in combination for the MOP system. In addition, based on the screened results, 21 new solid phases of MOP were experimentally observed. Among them, the crystal structures of 10 multicomponent crystals (cocrystals and salts) were revealed by single crystal X-ray diffraction analysis (SCXRD), and their thermodynamic and spectroscopy properties were also characterized. The Hirshfeld surface analysis and the molecular electrostatic potential (MEP) surface analysis were conducted to explore the interactions in multicomponent crystals and the origin for salts and cocrystals. The cases in this study not only enriched the solid forms of MOP, evidenced the feasibility of the combined screening method, but also set an effective example for choosing potential coformers to prepare multicomponent crystals.
研究领域:
药学
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材料科学
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晶体学
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物理化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）