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Nano Energy · 2019 · IF 15.548

Principle of proximity: Plasmonic hot electrons motivate donator-adjacent semiconductor defects with enhanced electrocatalytic hydrogen evolution

Bang Lin Li,Hao Lin Zou,Jie Kang Tian,Guo Chen,Xiao Hu Wang,Huan Duan,Xiao Lin Li,Yan Shi,Jing Rong Chen,Ling Jie Li,Jing Lei Lei,Hong Qun Luo,Nian Bing Li

Defects in layered semiconductors cause large variation of electric and catalysis properties, and exploiting defect-involved reaction can deeply excavate unearthed characteristics with significant performances. Mo-terminated defects of MoS 2 spontaneously guide the oriented growths of ultrasmall Au nanocrystals on specific sites of liquid-exfoliated (LE) nanosheets , which are experimentally and theoretically performed with programmable heterostructures . The conjugated construction of Au plasmonics and MoS 2 semiconductors is manipulated with the aim of the optimal synergistic activity. Additionally, with photonic irradiation, hot electrons excited from attached plasmonic nanostructures are injected into MoS 2 semiconductors, which remarkably increases the carrier density of catalyst to match the energy level of hydrogen evolution reaction (HER). Obeying the principle of proximity, localized MoS 2 defect-adjacent Au plasmonics exhibit a more valid pathway, transferring hot electrons from donators to receptors of catalytic sites, in comparison to planar Au decoration. Meanwhile, Au nanostructures located at basal planes are essential for accelerated electron transport rates between catalysts and electrodes, and high stabilities in plasmonic-motivated electrocatalytic performances are guaranteed. The dual function of location-discriminated Au nanostructures accounts for superior electrocatalytic HER performances with photonic excitation, which imparts high inspiration in expanded heterostructures and integrated plasmonic techniques for catalysis and devices.

CAS / MDL: 16961-25-4 361-09-1
研究领域: 材料科学 · 纳米技术 · 催化化学
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ACS Catalysis · 2021 · IF 13.084

Activating Edge-Mo of 2H-MoS2 via Coordination with Pyridinic N–C for pH-Universal Hydrogen Evolution Electrocatalysis

Jiayi Qin,Cong Xi,Rui Zhang,Tao Liu,Peichao Zou,Deyao Wu,Qianjin Guo,Jing Mao,Huolin Xin,Jing Yang

It is highly desirable to develop all-pH-compatible hydrogen evolution reaction (HER) electrocatalysts that can be used universally in a variety of different electrolyzers and operated in different pH conditions, i.e., acid, alkaline, microbial, chlor-alkali, etc. So far, two-dimensional layered MoS2 and Mo-based carbon materials have been regarded as promising pH-universal HER electrocatalysts. 2H-MoS2 as a naturally occurring and thermodynamically favorable phase, yet still suffers from poor HER activity in neutral and alkaline electrolytes. Herein, a hybrid electrocatalyst, i.e., 2H-MoS2/N-doped mesoporous graphene, rich in interfacial Mo–pyridinic N coordination is fabricated. The optimized hybrid catalyst delivers long-term durability and outstanding HER activity with overpotentials of 110, 145, and 142 mV at 10 mA cm–2 in acidic, alkaline, and phosphate buffered solutions (PBS) media, respectively, outperforming most of the previously reported MoS2-based catalysts. Theoretical and experimental results demonstrate that the interfacial pyridinic N has a higher tendency to bond with Mo atoms than pyrrolic and graphitic N, and the edge-Mo coordinated with pyridinic N could serve as HER active sites. DFT calculations further reveal that Mo–pyridinic N coordination modifies the charge density of edge-Mo, in turn optimizing the hydrogen absorption energy and facilitating water dissociation, and thereby significantly promoting the intrinsic catalytic activity for the pH-universal HER process.

研究领域: 材料科学 · 电化学 · 催化科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Synergistic enhancement of hydrogen evolution reaction by one-step pyrolysis synthesis of 1T-2H MoS2 loaded nitrogen-doped carbon

Jiabo Wang,Zhentao Liu,Wenxin Wang,Li Chen

The increasing demand for clean and renewable energy underscores the importance of hydrogen energy, with electrocatalytic water splitting being an efficient method for green hydrogen production. Platinum, while an excellent catalyst for hydrogen evolution reactions (HER), is hindered by high cost and scarcity. This study explores non-precious alternatives, focusing on MoS 2 due to its “platinum-like behavior.” The 1T-2H MoS 2 loaded on N-doped carbon (NC) catalysts (1T-2H MoS 2 @NC) were synthesized through a one-step pyrolysis of melamine and ammonium thiomolybdate. Comprehensive analysis revealed that the 2H phase formed at 700 °C, transitioning to a biphasic 1T-2H composition at higher temperatures. The catalyst synthesized at 800 °C with a 1:8 reactant ratio demonstrated exceptional HER performance, with an overpotential of 175 mV at 10 mA cm −2 and a Tafel slope of 92.37 mV dec −1 . This study highlights the potential of 1T-2H MoS 2 @NC as a cost-effective and efficient catalyst for sustainable hydrogen production.

CAS / MDL: 15060-55-6 108-78-1
研究领域: 材料科学 · 能源化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2023 · IF 7.2

MOF-derived MoS2@o-CoSe2 hetero-catalysts accompanied by structural phase transition for efficient electrochemical hydrogen production

Zongli Liu,Tian Wang,Pu Chang,Lixiu Guan,Xiaohu Wang,Chao Xu,Yingxuan Cao,Junguang Tao

Although electrocatalytic water splitting is a very promising and sustainable method for generating hydrogen as a clean energy source, the design and synthesis of stable and efficient noble metal-free catalysts faces some serious challenges. In this work, an electrocatalyst with heterostructure of MoS 2 and orthogonal phase of CoSe 2 (MoS 2 @o-CoSe 2 ) is derived from Co-based metal organic framework (Co-MOF). The complex shows excellent hydrogen evolution reaction (HER) activity and long-term stability in alkaline medium attributed to its porous structure , ultrathin nanosheet morphology, synergistic effect of each component owing to the tightly bonded interface and optimal electronic structure after phase transition. MoS 2 @o-CoSe 2 exhibits low overpotential of 34 mV at a current density of 10 mA cm −2 and a Tafel slope of 41 mV dec −1 . These results are superior to most recently reported Mo-based and Co-based electrocatalysts. Importantly, the performance of MoS 2 @o-CoSe 2 at high current densities is even better than that of commercial Pt/C electrode. Our results emphasize the importance of phase engineering and show that the combination of MOF with transition metal disulfides is an effective way to develop highly active and sustainable efficient electrocatalysts for water hydrolysis.

研究领域: 材料科学 · 能源化学
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Small · 2025 · IF 12.1

1D Co6Mo6C-Based Heterojunctional Nanowires from Pyrolytically “Squeezing” PMo12/ZIF-67 Cubes for Efficient Overall Water Electrolysis

Xinhui Zhang,Aiping Wu,Dongxu Wang,Ying Xie,Aleksandr I. Gubanov,Gennadiy A. Kostin,Chungui Tian

The bi-transition-metal interstitial compounds (BTMICs) are promising for water electrolysis. The previous BTMICs are usually composed of irregular particles. Here, this work shows the synthesis of novel 1D Co 6 Mo 6 C-based heterojunction nanowires (1D Co/Co 6 Mo 6 C) with diameters about 50 nm and a length-to-diameter ratio about 20 for efficient water electrolysis. An interesting growth process based on pyrolytically “squeezing” PMo 12 (Phosphomolybdic acid)/ZIF-67 (Zeolitic Imidazolate Framework-67) cube precursor is demonstrated. The “squeezing” growth is related to the role of Mo species for isolating Co species. A series of tests and theoretical calculation show the mutual regulation of Co and Mo to optimize the electronic structure, accelerating H 2 O dissociation and the reduction kinetics of H + . Additionally, the nanowires provide pathways for electron transfer and the transmission of reactants. Consequently, the 1D Co/Co 6 Mo 6 C exhibits high activity for hydrogen evolution reaction ( η 10 of 31 mV) and oxygen evolution reaction ( η 10 of 210 mV) in 1 m KOH. The electrolytic cell based on 1D Co/Co 6 Mo 6 C requires a low voltage of 1.43 V to drive 10 mA cm −2 . The catalyst also exhibits good HER performance in 1 m phosphate-buffered saline solution, exceeding Pt/C at a current density >42 mA cm −2 .

研究领域: 材料科学 · 电化学 · 催化反应
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Nanomaterials · 2023 ·Vol. 13 ·期 16 ·2302 · IF 5.3

Construction of an Amethyst-like MoS2@Ni9S8/Co3S4 Rod Electrocatalyst for Overall Water Splitting

Zhen Pei,Tengteng Qin,Rui Tian,Yangxin Ou,Xingzhong Guo

Transition metal sulphide electrocatalytic materials possess the bright overall water-splitting performance of practical electrocatalytic technologies. In this study, an amethyst-like MoS2@Ni9S8/Co3S4rod electrocatalyst was constructed via a one-step hydrothermal method with in-situ-grown ZIF-67 nanoparticles on nickel foam (NF) as a precursor. The rational design and synthesis of MoS2@Ni9S8/Co3S4endow the catalyst with neat nanorods morphology and high conductivity. The MoS2@Ni9S8/Co3S4/NF with the amethyst-like rod structure exposes abundant active sites and displays fast electron-transfer capability. The resultant MoS2@Ni9S8/Co3S4/NF exhibits outstanding hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) electrocatalytic activities, with low overpotentials of 81.24 mV (HER) at 10 mA cm−2and 159.67 mV (OER) at 50 mA cm−2in 1.0 M KOH solution. The full-cell voltage of overall water splitting only achieves 1.45 V at 10 mA cm−2. The successful preparation of the amethyst-like MoS2@Ni9S8/Co3S4rod electrocatalyst provides a reliable reference for obtaining efficient electrocatalysts for overall water splitting.

研究领域: 材料科学 · 电化学
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES · 2019 ·Vol. 35 ·期 2 ·179-185 · IF 1.071

Hydrothermal Synthesized Co-Ni3S2 Ultrathin Nanosheets for Efficient and Enhanced Overall Water Splitting

Jian Juan,Yuan Long,Li He,Liu Huanhuan,Zhang Xinghui,Sun Xuejiao,Yuan Hongming,Feng Shouhua

We used the one-step hydrothermal controlled synthesis method for Co-Ni 3 S 2 ultrathin nanosheets grown directly on nickel foam(NF). The as-synthesized Co-Ni 3 S 2 /NF showed enhanced activities in the hydrogen evolution reaction(HER), oxygen evolution reaction(OER) and better overall water splitting(OWS) efficiency than the un-doped Ni 3 S 2 /NF. The voltage of Co-Ni 3 S 2 /NF for OWS was only 1.58 V at the current density of 10 mA/cm 2 and with long time(>30 h) current output during the current-density( i - t ) test. The good i - t performance was also observed in both HER and OER processes. Additionally, the Co-Ni 3 S 2 /NF showed a large current density(>1 A/cm 2 ) for both HER and OER. When the current densities reached 100 and 1000 mA/cm 2 , the required overpotentials for Co-Ni 3 S 2 /NF were 0.35 and 0.75 V for OER and 0.30 and 0.85 V for HER. Therefore, after introducing Co, th e activity of Ni 3 S 2 -based material was strongly enhanced.

研究领域: 材料科学 · 能源化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Chemical dealloying derived nanoporous FeCoNiCuTi high-entropy bifunctional electrocatalysts for highly efficient overall water splitting under alkaline conditions

Yezeng He,Jiaojiao Qin,Fangyu Hu,Liang Mao,Baolong Shen,Tejraj M. Aminabhavi,Yasser Vasseghian,Akbar Hojjati-Najafabadi

In response to society’s urgent drive to significantly decrease its reliance on fossil fuels in the future, there has been continuing efforts to utilize hydrogen (H 2 ) generated by water electrolysis as clean and sustainable substitute for the traditional fossil fuels. A significant challenge in water electrolysis revolves around creating affordable and efficient electrocatalysts to speed up the chemical reactions involved. Our new study introduces a bifunctional catalyst made from a high-entropy alloy (HEA), capable of efficiently catalyzing both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). The findings reveal that a complex chemical composition of FeCoNiCuTi HEA can significantly modify its electronic structure, resulting in an impressive electrocatalytic performance. Specifically, FeCoNiCuTi HEA catalyst exhibits an overpotential of 64.9 mV at a current density of 10 mA cm −2 for hydrogen evolution with a Tafel slope of 36.81 mV dec −1 and double-layer capacitance ( C dl ) of 34.1 mF cm −2 . For oxygen evolution, HEA achieves an overpotential of 175 mV at 10 mA cm −2 , a Tafel slope of 44.31 mV dec −1 , exhibiting the performance superior to noble catalysts. Theoretical calculations support that the intricate chemical composition of high-entropy alloy plays vital role to enhance its electrocatalytic capabilities. This research represents a straightforward efficient method to create electrocatalysts for water electrolysis using non-noble metals by leveraging high-entropy effect.

CAS / MDL: 7647-01-0
研究领域: 材料科学 · 化学
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RSC Advances · 2015 ·Vol. 5 ·期 110 ·90265-90271 · IF 3.84

MOF-derived nanostructured cobalt phosphide assemblies for efficient hydrogen evolution reaction

Lili Li,Xingyue Li,Lunhong Ai,Jing Jiang

The earth-abundant metal phosphides have emerged as new and active alternatives for the precious metal platinum to electrocatalyze the hydrogen evolution reaction (HER) via water splitting. In this study, we report on the straightforward and controllable synthesis of various nanostructured cobalt phosphide assemblies through the direct chemical transformation of a Co-containing metal–organic framework (ZIF-67-Co) under mild phosphorization conditions. The resulting CoP nanoparticle assemblies (NPAs) and nanorod assemblies (NRAs) can be selectively produced by rationally tuning the calcination atmosphere. The CoP NRAs were found to be highly active for electrocatalytic hydrogen generation, which exhibited better performance than that of the CoP NPAs, as evidenced by their relatively low onset overpotential (∼86 mV), small Tafel slope (∼69 mV dec−1) and long-term stability in acidic media.

CAS / MDL: 693-98-1 7681-53-0
研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2018 · IF 5.116

Molybdenum carbide in-situ embedded into carbon nanosheets as efficient bifunctional electrocatalysts for overall water splitting

Jiangnan Xing,Yang Li,Siwei Guo,Ting Jin,Haixia Li,Yijing Wang,Lifang Jiao

Developing low-cost and highly efficient electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is attractive for overall water splitting. Herein, we firstly use the globally generated green cornstalks as the carbon source to prepare highly efficient bifunctional pure β-phase molybdenum carbide (β-Mo 2 C) electrocatalysts . Due to the highly intrinsic activity of β-Mo 2 C, high porosity of the resultant and synergistic effect between the Mo 2 C and carbon matrix, the as-prepared catalyst exhibits excellent electrocatalytic activities with low overpotentials of 130 mV and 274 mV to achieve a current density of 10 mA cm −2 for the HER and OER, respectively. As a bifunctional electrocatalyst for overall water splitting, the electrolyzer only needs a cell voltage of 1.65 V at 10 mA cm −2 in alkaline water, as well as long-term stability of 30 h. This intriguing preparation strategy will open up an exciting new avenue for the synthesis of other carbides.

CAS / MDL: 12030-49-8 1310-58-3
研究领域: 材料科学 · 能源科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

CoNi-phosphides with iron incorporation effectively boost hydrogen evolution reaction and oxygen evolution reaction for overall water splitting

Yifan Kuang,Shuang Zhao,Shang Gao,Na Song

Rational design of high-efficiency, durable and cost-effective electrocatalysts for H 2 production is essential to accelerate hydrogen production from fundamental experiments to practical industrial applications. Herein, cobalt-nickel-iron phosphides are constructed on Ni foam (CoNiFeP@NF) via a simple one-step electrochemical deposition method as self-supported electrodes for efficiently water splitting. The introduction of Fe element significantly enhances the catalytic properties of CoNiP@NF electrode for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Additionally, the optimal HER and OER electrodes are obtained by adjusting the Fe 3+ concentration at 0.1 ( [email protected] ) and 0.15 M ( [email protected] ), respectively. Benefiting from the modulation of the electronic structure of CoNiP by the Fe element, [email protected] and [email protected] electrodes only require the overpotentials (η) of 48 mV for HER and 223 mV for OER to reach the current density of 10 mA cm −2 , superior to the reference CoNiP@NF electrode (η 10, HER  = 89 mV, η 10, OER  = 333 mV). Subsequently, the electrolyzer constructed by [email protected] as cathode and [email protected] as anode exhibits excellent overall water splitting performance with a cell voltage of 1.56 V at a current density of 10 mA cm −2 . This work provides a convenient and effective strategy for regulating the catalytic activity of bifunctional phosphide catalysts for water splitting.

研究领域: 材料科学 · 能源化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Self-supported tungsten-doped nickel-iron layered phosphides for efficient electrocatalytic alkaline water splitting

Ling-Xin Kong,Hui-Hao Li,Xin-Qi Liu,Xin-Jie Ni,Mei-Ling Xue,Yi Fang,Ji-Sen Li,Shan Huang,Qi Xiao

Although layered double hydroxides (NiFe-LDH) have demonstrated adequate oxygen evolution reaction (OER) performance since their inception, their low hydrogen evolution performance has traditionally limited their application in overall water splitting (OWS). In this study, FeWO 4 @Ni 2 P/FeNiP (NiFeW-P) self-supported nanosheets were grown on NF (NiFeW-P@NF) using cation doping and subsequent anion exchange processes. NiFeW-P@NF with lower crystallinity exhibited more corners and edges, thereby exposing numerous catalytic active sites and greatly improving both oxygen and hydrogen evolution performance. Excellent electrocatalytic hydrogen evolution reaction (HER) and OER activity were demonstrated by the produced NiFeW-P@NF catalysts, achieving reaction current densities of 10 mA·cm −2 with overpotentials of just 81 mV and 174 mV, respectively. Moreover, they exhibited stability for over 100 hours at current densities around 1000 mA·cm −2 . When assembled into an alkaline electrolyzer, NiFeW-P@NF sustained an OWS current density of approximately 1200 mA·cm −2 for more than 100 h at just 1.48 V. This work sheds more light on the evolution of NiFe-LDH's enhanced electrocatalytic OWS characteristics.

研究领域: 材料科学 · 电化学
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