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Journal Article•DOI•

An acid-base molecular assembly strategy toward N-doped Mo2C@C nanowires with mesoporous Mo2C cores and ultrathin carbon shells for efficient hydrogen evolution.

Qiqi Jing1, Jiahui Zhu1, Xiangru Wei1, Yaqian Lin1, Xiaoning Wang1, Zhangxiong Wu1 •
15 Nov 2021-Journal of Colloid and Interface Science (Academic Press)-Vol. 602, pp 520-533
TL;DR: In this paper, an acid-base molecular assembly strategy is demonstrated for the synthesis of novel N-doped Mo2C@C core-shell nanowires (NWs) composed of mesoporous Mo 2C cores with interconnected crystalline walls and ultrathin carbon shells.
About: This article is published in Journal of Colloid and Interface Science.The article was published on 2021-11-15. It has received 13 citations till now. The article focuses on the topics: Mesoporous material & Overpotential.
Citations
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Journal Article•DOI•
TL;DR: In this paper , N-doped nanoparticles self-encoded in nanospheres are presented as a highperforming HER electrocatalyst fabricated through a one-pot solvothermal method followed by hydrogen calcination.

19 citations

Journal Article•DOI•
TL;DR: In this article , the authors proposed a novel strategy to construct Mo2N uniformly embedded Mo2C nanobelt arrays electrocatalyst on N doped carbon framework (Mo2N-Mo2C/NC NBAs) by nitridation of MoOx/C hybrid precursors and subsequent annealing.

7 citations

Journal Article•DOI•
TL;DR: In this paper , a facile strategy was proposed to prepare Mo-precursor by coordination of Mo with polysaccharide from natural biomass (jujube), which also acted as carbon and chelating agent.

5 citations

Journal Article•DOI•
TL;DR: In this article , the surface doping effect on electrocatalytic hydrogen evolution reaction (HER) was investigated by density functional theory (DFT), and the thermodynamical stability and realistic catalytic surface of doped surfaces, including mono-and co-doping by three elements with various doping ratios, were verified by formation energies and surface Pourbaix diagrams, respectively.

5 citations

Journal Article•DOI•
TL;DR: In this paper , a rational design of Co-Co0.85Se heterostructures anchoring on the defective N-doped carbon matrix is obtained from hydrothermal-carbonization process of pectin, melamine and cobalt chloride.

3 citations

References
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Journal Article•DOI•
TL;DR: This review highlights the recent research efforts toward the synthesis of noble metal-free electrocatalysts, especially at the nanoscale, and their catalytic properties for the hydrogen evolution reaction (HER), and summarizes some important examples showing that non-Pt HER electrocatsalysts could serve as efficient cocatalysts for promoting direct solar-to-hydrogen conversion in both photochemical and photoelectrochemical water splitting systems, when combined with suitable semiconductor photocatalyst.
Abstract: Sustainable hydrogen production is an essential prerequisite of a future hydrogen economy. Water electrolysis driven by renewable resource-derived electricity and direct solar-to-hydrogen conversion based on photochemical and photoelectrochemical water splitting are promising pathways for sustainable hydrogen production. All these techniques require, among many things, highly active noble metal-free hydrogen evolution catalysts to make the water splitting process more energy-efficient and economical. In this review, we highlight the recent research efforts toward the synthesis of noble metal-free electrocatalysts, especially at the nanoscale, and their catalytic properties for the hydrogen evolution reaction (HER). We review several important kinds of heterogeneous non-precious metal electrocatalysts, including metal sulfides, metal selenides, metal carbides, metal nitrides, metal phosphides, and heteroatom-doped nanocarbons. In the discussion, emphasis is given to the synthetic methods of these HER electrocatalysts, the strategies of performance improvement, and the structure/composition-catalytic activity relationship. We also summarize some important examples showing that non-Pt HER electrocatalysts could serve as efficient cocatalysts for promoting direct solar-to-hydrogen conversion in both photochemical and photoelectrochemical water splitting systems, when combined with suitable semiconductor photocatalysts.

4,351 citations

Journal Article•DOI•
TL;DR: This work couple graphitic-carbon nitride with nitrogen-doped graphene to produce a metal-free hybrid catalyst, which shows an unexpected hydrogen evolution reaction activity with comparable overpotential and Tafel slope to some of well-developed metallic catalysts.
Abstract: Electrocatalytic reduction of water to molecular hydrogen via the hydrogen evolution reaction may provide a sustainable energy supply for the future, but its commercial application is hampered by the use of precious platinum catalysts. All alternatives to platinum thus far are based on nonprecious metals, and, to our knowledge, there is no report about a catalyst for electrocatalytic hydrogen evolution beyond metals. Here we couple graphitic-carbon nitride with nitrogen-doped graphene to produce a metal-free hybrid catalyst, which shows an unexpected hydrogen evolution reaction activity with comparable overpotential and Tafel slope to some of well-developed metallic catalysts. Experimental observations in combination with density functional theory calculations reveal that its unusual electrocatalytic properties originate from an intrinsic chemical and electronic coupling that synergistically promotes the proton adsorption and reduction kinetics.

1,774 citations

Journal Article•DOI•
TL;DR: The fundamentals of HER are summarized and the recent state-of-the-art advances in the low-cost and high-performance catalysts based on noble and non-noble metals, as well as metal-free HER electrocatalysts are reviewed.
Abstract: Hydrogen fuel is considered as the cleanest renewable resource and the primary alternative to fossil fuels for future energy supply. Sustainable hydrogen generation is the major prerequisite to realize future hydrogen economy. The electrocatalytic hydrogen evolution reaction (HER), as the vital step of water electrolysis to H2 production, has been the subject of extensive study over the past decades. In this comprehensive review, we first summarize the fundamentals of HER and review the recent state-of-the-art advances in the low-cost and high-performance catalysts based on noble and non-noble metals, as well as metal-free HER electrocatalysts. We systemically discuss the insights into the relationship among the catalytic activity, morphology, structure, composition, and synthetic method. Strategies for developing an effective catalyst, including increasing the intrinsic activity of active sites and/or increasing the number of active sites, are summarized and highlighted. Finally, the challenges, perspectives, and research directions of HER electrocatalysis are featured.

1,387 citations

Journal Article•DOI•
Jing Wang1, Fan Xu1, Haiyan Jin1, Yiqing Chen1, Yong Wang1 •
TL;DR: A detailed analysis of the structure-activity-pH correlations in the HER process gives an insight on the origin of the pH-dependence for HER, and provides guidance for future HER mechanism studies on non-noble metal-based carbon composites.
Abstract: Hydrogen has been hailed as a clean and sustainable alternative to finite fossil fuels in many energy systems. Water splitting is an important method for hydrogen production in high purity and large quantities. To accelerate the hydrogen evolution reaction (HER) rate, it is highly necessary to develop high efficiency catalysts and to select a proper electrolyte. Herein, the performances of non-noble metal-based carbon composites under various pH values (acid, alkaline and neutral media) for HER in terms of catalyst synthesis, structure and molecular design are systematically discussed. A detailed analysis of the structure-activity-pH correlations in the HER process gives an insight on the origin of the pH-dependence for HER, and provide guidance for future HER mechanism studies on non-noble metal-based carbon composites. Furthermore, this Review gives a fresh impetus to rational design of high-performance noble-metal-free composites catalysts and guide researchers to employ the established electrocatalysts in proper water electrolysis technologies.

1,258 citations

Journal Article•DOI•
Hao Bin Wu1, Bao Yu Xia1, Le Yu1, Xin-Yao Yu1, Xiong Wen David Lou1 •
TL;DR: A metal-organic frameworks-assisted strategy for synthesizing nanostructured transition metal carbide nano-octahedrons composed of ultrafine nanocrystallites exhibited remarkable electrocatalytic performance for hydrogen production from both acidic and basic solutions is demonstrated.
Abstract: Electrochemical water splitting has been considered as a promising approach to produce clean and sustainable hydrogen fuel. However, the lack of high-performance and low-cost electrocatalysts for hydrogen evolution reaction hinders the large-scale application. As a new class of porous materials with tunable structure and composition, metal-organic frameworks have been considered as promising candidates to synthesize various functional materials. Here we demonstrate a metal-organic frameworks-assisted strategy for synthesizing nanostructured transition metal carbides based on the confined carburization in metal-organic frameworks matrix. Starting from a compound consisting of copper-based metal-organic frameworks host and molybdenum-based polyoxometalates guest, mesoporous molybdenum carbide nano-octahedrons composed of ultrafine nanocrystallites are successfully prepared as a proof of concept, which exhibit remarkable electrocatalytic performance for hydrogen production from both acidic and basic solutions. The present study provides some guidelines for the design and synthesis of nanostructured electrocatalysts. There is extensive research into non-platinum electrocatalysts for hydrogen evolution. Here, the authors report a molybdenum carbide catalyst, prepared via the carburization of a copper metal-organic framework host/molybdenum-based polyoxometalates guest system, and demonstrate its catalytic activity.

1,194 citations

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