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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES · 2022 ·Vol. 23 ·期 13 ·7477 · IF 6.208

Laser Shock Fabrication of Nitrogen Doped Inverse Spinel Fe3O4/Carbon Nanosheet Film Electrodes towards Hydrogen Evolution Reactions in Alkaline Media

Dun Wu,Jiaming Zhao,Junfeng Cheng,Chunlin Liu,Qiang Wang

The reliable and cost-effective production of high-performance film electrodes for hydrogen evolution reactions remains a challenge for the laser surface modification community. In this study, prior to a thermal imidization reaction, a small number of Fe3O4nanoparticles were vortexed into a poly(amic acid) (PAA) prepolymer, and the achieved flat composite film was then ablated by a 1064 nm fiber laser. After laser irradiation, the hierarchical architectures of carbon nanosheets decorated with Fe3O4nanoparticles were generated. Although pure polyimide (PI) film and laser carbonized PI film, as well as bare Fe3O4, showcase poor intrinsic catalytic activity toward alkaline hydrogen evolution reactions, our laser-derived Fe3O4/carbon nanosheet hybrid film demonstrated enhanced electrocatalytic activity and stability in 1 M KOH electrolyte; the overpotential(η10) reached 247 mV when the current density was 10 mA cm−2with a slight current decay in the chronoamperometric examination of 12 h. Finally, we proposed that the substitution of N to O in Fe−O sites of trans spinel structured magnetite would be able to modulate the free energy of hydrogen adsorption (ΔGH*) and accelerate water dissociation.Keywords:laser ablation;photothermal agent;hydrogen evolution reaction

研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Defect-Driven hydrogen Evolution: Enhanced hydrogen spillover on Pt-MoS2 interface via sulfur vacancies

Juan Du,Tianfeng Cai,Qiao Han,Hongda Wu,Qing Zhao,Lufan Zheng,Shuo Liu,Zhanxu Yang

The hydrogen spillover is considered a powerful strategy for improving the kinetics of hydrogen evolution reaction (HER) due to the decoupling of hydrogen adsorption and desorption. However, the hydrogen spillover rate strongly depends on the metal-support interfaces, and the Fermi levels (E f ) difference between metal and support hinders the occurrence of hydrogen spillover. Here, we prepared platinum (Pt) doped on molybdenum disulfide (MoS 2 ) with sulfur vacancies (Sv) catalyst (Pt/Sv-MoS 2 ) and investigated the internal relationship between metal-support interfaces and hydrogen spillover mechanism. The experimental and theoretical results show that sulfur (S) vacancies reduce the work function (ΔΦ) at the metal-support interface, thus accelerating the migration rate of hydrogen from Pt to Sv-MoS 2 . Meanwhile, the introduction of S vacancies promotes the high dispersion of Pt nanoparticles (Pt NPs) and weakens the electron supply from Pt to MoS 2 , facilitating active hydrogen (*H) adsorption step and thus increasing the hydrogen coverage on the Pt sites. Consequently, the prepared Pt/Sv-MoS 2 catalyst exhibited significantly enhanced HER activity, achieving an overpotential of 26 mV at 10 mA·cm −2 and a Tafel slope of only 28 mV·dec −1 , which is superior to commercial 20 % Pt/C.

研究领域: 材料科学 · 催化化学
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Materials Horizons · 2017 ·Vol. 5 ·期 1 ·108-115 · IF 10.706

Co/CoP embedded in a hairy nitrogen-doped carbon polyhedron as an advanced tri-functional electrocatalyst

Yongchao Hao,Yuqi Xu,Wen Liu,Xiaoming Sun

The design and synthesis of a multi-functional electrocatalyst with low cost and high efficiency is still a great challenge. Herein, we report the rational design and realization of a tri-functional electrocatalyst featuring Co/CoP embedded in a hairy nitrogen-doped carbon polyhedral (Co/CoP–HNC) derived from common metal organic frameworks (MOFs). The components of Co, CoP, and hairy nitrogen-doped carbon in the catalyst respectively render catalytic activity, high electrochemical surface area, and electronic conductivity. The synergy of the tailored Co/CoP–HNC catalyst provides high activity for oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). The catalytic performance and assembly feasibility are further demonstrated in overall water splitting and Zn–air battery tests, and both revealed high efficiency and long durability of the proposed electrocatalyst.

研究领域: 材料科学 · 能源化学 · 催化化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Oxygen vacancies and interfacial engineering of RuO2/CeO2-NC heterojunction for pH-universal hydrogen evolution reaction

Jihan Wu,Ying Chang,Shaohong Guo,Aiju Xu,Jingchun Jia,Meilin Jia

Ruthenium-based nanomaterials are considered to be promising electrocatalysts for HER due to their higher activity. However, the active site exposure is low, and the catalytic mass activity is low. In order to achieve the particular aims, several types of engineering, such as crystal engineering, topography engineering, heterostructures and support engineering, have been used to catalysts. Here we report RuO 2 supported on CeO 2 -NC, owing to the abundant heterostructures and the presence of oxygen vacancies, the RuO 2 /CeO 2 -NC catalyst showed outstanding HER performance (98.2 mV, 53 mV and 298 mV@100 mA cm −2 in acidic, alkaline and neutral, respectively). Moreover, RuO 2 /CeO 2 -NC also has an excellent electrocatalytic durability for 40 h. The experimental achievements show that oxygen vacancies and heterostructures could jointly enhance performance of catalyst HER.

研究领域: 材料科学 · 电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Edge-oriented, high-percentage 1T′-phase MoS2 nanosheets stabilize Ti3C2 MXene for efficient electrocatalytic hydrogen evolution

Xitao Li,Xinding Lv,Xiangnan Sun,Chen Yang,Yan-Zhen Zheng,Lihui Yang,Siqi Li,Xia Tao

Abundant electrochemical active sites, high electronic conductivity as well as stable structure and electrochemical activity are indispensable but usually incompatible to the ideal electrocatalysts for hydrogen evolution reaction (HER). Herein, an efficient and stable MoS 2 -Ti 3 C 2 MXene electrocatalyst is synthesized using a delicately designed one-step hydrothermal method, in which the few-layers thick, edge-oriented, high-percentage 1T′-phase (∼ 85.0 %) MoS 2 nanosheets are well grown on the cation-modified Ti 3 C 2 MXene and stabilize Ti 3 C 2 MXene against spontaneous oxidation caused by dissolved-oxygen. The structure and phase engineering of MoS 2 as well as the fully surface-shielding Ti 3 C 2 MXene endow the as-synthesized MoS 2 -Ti 3 C 2 MXene electrocatalyst with a wealth of accessible active sites and high electrical conductivity for HER together with excellent structure stability. Consequently, the as-synthesized MoS 2 -Ti 3 C 2 MXene exhibits remarkable electrocatalytic HER performance in acidic medium with a low overpotential of 98 mV at 10 mA cm -2 , a depressed Tafel slope of 45 mV dec -1 and a low electrochemical resistance.

研究领域: 材料科学 · 电化学
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NEW JOURNAL OF CHEMISTRY · 2019 ·Vol. 43 ·期 10 ·4160-4167 · IF 3.069

Facile synthesis of porous carbon/Ni12P5 composites for electrocatalytic hydrogen evolution

Fangxiao Wang,Yan-ming Liu,Chun-yang Zhang

Water splitting into hydrogen (H2) to produce clean energy is of great significance for sustainable development. Transition metal phosphides (e.g., Ni12P5 nanoparticles) may be used as non-precious earth-abundant electrocatalysts for the H2 evolution reaction, but their poor electronic conductivity and small surface area hinder efficient catalytic H2 production. In this research, we demonstrate for the first time the facile synthesis of porous carbon/Ni12P5 (C/NiP-C) composites with the dispersion of Ni12P5 nanoparticles onto a conductive porous carbon support in an ionic surfactant hexadecyl trimethyl ammonium bromide (CTAB)-mediated ethanol solution. The CTAB plays dual roles in the synthesis including (1) the introduction of carbon to increase the conductivity of the synthetic materials and (2) the formation of uniform Ni12P5 phosphides through the interaction between the H2PO2− anion, Ni2+, and C19H42N+ cation dissociated from CTAB. The obtained C/NiP-C composites may function as electrocatalysts for the hydrogen evolution reaction (HER) with excellent HER performance (η: 63 mV, η10: 176 mV, Tafel slope: 100 mV dec−1, wherein η represents the onset overpotential and η10 represents the overpotential required for a current density (j) value of −10 mA cm−2) compared with the NixPy composites synthesized in pure ethanol (η: 160 mV, η10: 392 mV, Tafel slope: 154 mV dec−1), the C/NiP-P composites synthesized in a P123-mediated ethanol solution (η: 75 mV, η10: 286 mV, Tafel slope: 210 mV dec−1), and the C/NiP-F composites synthesized in a F127-mediated ethanol solution (η: 80 mV, η10: 302 mV, Tafel slope: 189 mV dec−1). The enhanced HER performance can be attributed to the synergistic effects resulting from the unique structure of the porous C support and the well dispersed Ni12P5 nanoparticles.

CAS / MDL: 7681-53-0
研究领域: 材料科学 · 电化学
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ChemSusChem · 2019 ·Vol. 12 ·期 7 ·1368-1373 · IF 7.804

Oxygen-Functionalized Ultrathin Ti3C2Tx MXene for Enhanced Electrocatalytic Hydrogen Evolution

Yanan Jiang,Tao Sun,Xi Xie,Wei Jiang,Jia Li,Bingbing Tian,Chenliang Su

Graphical S‘O’ much win with MXene : A facile method is reported to produce ultrathin Ti 3 C 2 MXene functionalized with oxygen as an electrocatalyst for the hydrogen evolution reaction. The terminal O on the basal plane increases the number of active sites for electrocatalysis. This combined with the high surface area and conductivity enables the O-functionalized MXene to show enhanced electrocatalytic performance for hydrogen evolution. Two-dimensional (2D) transition-metal carbides (MXenes) are widely adopted as potential electrocatalysts for the hydrogen evolution reaction (HER) owing to their metallic conductivity, rich tunable surface chemistry, and atomic thickness with highly exposed active sites. Previously published theoretical results indicate that MXenes functionalized entirely with oxygen have lower Δ G H* for HER. However, MXenes contain many terminal F groups on the basal plane, which is detrimental to the HER. Herein, the development of an ultrathin Ti 3 C 2 MXene nanosheet fully functionalized with oxygen is reported for the HER. The obtained oxygen-functionalized Ti 3 C 2 (Ti 3 C 2 O x ) exhibits a much higher HER activity (190 mV at 10 mA cm −2 ) than that of Ti 3 C 2 T x (T=F, OH, and O). The improved HER performance is attributed to the highly active O sites on the basal plane of Ti 3 C 2 T x MXenes. This study paves way for electrocatalytic applications of MXene materials by tuning their surface functional groups.

CAS / MDL: 7664-39-3
研究领域: 材料科学 · 电化学
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Functional Materials Letters · 2024 · IF 1.2

Ruthenium-doped Ni5P4 for hydrogen production via water electrolysis

Yaoting Wang,Zhiling Chou,Huimin Zhang,Yiming Zou,Junfu Wang,Haochen Ding,Hong Zhao,Song Wang,Xin Xiao

The electrochemical decomposition of water to produce hydrogen using clean energy sources has become a sustainable pathway for hydrogen utilization, with efficient hydrogen evolution reaction (HER) electrocatalysts crucial for high energy conversion efficiency. Nickel phosphide is widely utilized in the electrocatalytic HER owing to its unique electronic properties, efficient electrocatalytic performance, and excellent corrosion resistance. However, the HER activity of nickel–phosphide electrocatalysts remains low, necessitating further research for practical applications. This paper introduces a method for preparing Ru-doped Ni 5 P 4 , including the mechanism of the HER, the preparation of Ru@Ni 5 P 4 , and its performance in electrocatalytic hydrogen evolution. The preparation methods for the Ru@Ni 5 P 4 electrocatalyst were classified, with a focus on the preparation techniques and research progress regarding its HER activity. The HER activities of the pure Ni 5 P 4 , Ru@Ni 5 P 4 , and 10 wt.% Pt/C electrodes were compared based on experimental indicators such as the overpotential and Tafel slope at a specific current density.

研究领域: 材料科学 · 电化学 · 能源化学 · 催化化学 · 可持续能源
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

Carbon dots-Pt modified polyaniline nanosheet grown on carbon cloth as stable and high-efficient electrocatalyst for hydrogen evolution in pH-universal electrolyte

Qian Dang,Yuyang Sun,Xiao Wang,Wenxiang Zhu,Ying Chen,Fan Liao,Hui Huang,Mingwang Shao

Design and fabrication of hydrogen evolution reaction (HER) electrocatalysts with high activity, durability and moderate price are vital for realizing a viable water-splitting technology. Here, we demonstrate the carbon dots-Pt modified polyaniline nanosheets grown on carbon cloth (CDs/Pt-PANI) can serve as stable and high-efficient electrocatalyst in pH-universal electrolyte for HER. The overpotential for optimal CDs/Pt-PANI electrocatalyst can be lowered to 30 mV at 10 mA·cm −2 when Pt loading was only 8.1 μg·cm −2 (the Pt content in commercial 20 wt% Pt/C is 22.4 μg·cm −2 ), showing exceptional HER efficiency with a small Tafel slope 41.7 mV·dec −1 in acidic solution. Meanwhile, the optimal CDs/Pt-PANI electrocatalyst exhibits well stability with 17 mV potential shift after 20 h, which is 0.06 times than that of commercial 20 wt% Pt/C (286 mV). It is noticeable, the optimal CDs/Pt-PANI electrocatalyst is superior to 20 wt% Pt/C with HER performance in pH-universal electrolyte (acidic, neutral and basic). The efficient and stable HER performance of CDs/Pt-PANI should ascribe to the synergy in the CDs, Pt and PANI, in which the surface functional groups of CDs can connect tightly with PANI and improve the stability of Pt, simultaneously, the PANI and Pt provide the high-efficiency in HER.

研究领域: 材料科学 · 电化学
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Nanoscale · 2024 ·Vol. 16 ·期 47 ·21947-21959 · IF 5.8

Interfacial coupling of NiSe in heterostructures promotes electrocatalytic hydrolysis of MoS2

Feng Jiao,Jun Tang,Jinzhao Huang,Zehui Liu,Jing Xiao

Molybdenum sulfide (MoS2) has attracted much attention as a potential catalyst for the oxygen evolution reaction (OER), but its unique low activity and low edge active centers limit its electrocatalytic activity. In this study, catalysts were prepared by growing NiSe nanoclusters in situ onto MoS2 substrates via electrodeposition; ultrathin MoS2 nanosheets and NiSe nanoclusters were cross-linked with each other to form a unique three-dimensional rosette structure; and MoS2@NiSe catalysts were successfully synthesised, which significantly improved bifunctional catalytic performance. The synthesised MoS2@NiSe catalysts exhibited good electrochemical performance: overpotentials required to satisfy the HER and OER processes at a current density of 10 mA cm−2 in 1 M KOH were 80 mV and 254 mV, respectively. When applied as a cathode and anode to assemble a bifunctional electrode system, the MoS2@NiSe||MoS2@NiSe electrolytic cell system required only 1.54 V to achieve 10 mA cm−2 in an alkaline electrolyte, which exceeded the value of most of the bifunctional catalysts reported in the literature to date. In addition, the catalyst maintained good surface structure and catalytic performance after a 24 h stability test. This study provides a new idea for the improvement and design of MoS2-based bifunctional catalysts and provides an important reference for research in the field of clean energy.

CAS / MDL: 7791-20-0
研究领域: 材料科学 · 能源化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

In-Situ and controllable construction of Mo2N embedded Mo2C nanobelts as robust electrocatalyst for superior pH-universal hydrogen evolution reaction

Hao Song,Siguang Guo,Xuming Zhang,Yixuan Yang,Biao Gao,Yuancheng Pi,Chaoran Pi,Paul K. Chu,Kaifu Huo

The development of high active and cost-effective transition metal based catalysts as alternatives to Pt-based electrocatalysts for pH-universal hydrogen evolution reaction (HER) is highly desirable. Herein, we proposed a novel strategy to construct Mo 2 N uniformly embedded Mo 2 C nanobelt arrays electrocatalyst on N doped carbon framework (Mo 2 N-Mo 2 C/NC NBAs) by nitridation of MoO x /C hybrid precursors and subsequent annealing. The effect of N content towards the composition ratio of Mo 2 N to Mo 2 C and the structural evolution were studied. The in-situ formed Mo 2 N reduces the sintering of Mo 2 C phase and creates amounts of compact Mo 2 N-Mo 2 C interfaces and mesopores. Because of these high active interfaces, mesopores structure and self-supported architecture, the resultant Mo 2 N-Mo 2 C/NC catalyst exhibits remarkable HER performance and durability over a wide pH range, as exemplified by a small overpotentials of 75, 93, and 114 mV at 10 mA cm −2 , and Tafel slopes of 43, 58, and 62 mV dec −1 in the alkaline, neutral and acidic media. The results reveal a new avenue to design highly efficient electrocatalysts with tailored hetero/microstructures, which could be extended to fabricate other high-performance electrocatalyst and electrode materials for electrochemical energy conversion.

研究领域: 材料科学 · 电化学 · 能源转换
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NANOTECHNOLOGY · 2020 ·Vol. 31 ·期 20 ·205604 · IF 3.551

Fabrication of hierarchical SrTiO3@MoS2 heterostructure nanofibers as efficient and low-cost electrocatalysts for hydrogen-evolution reactions

Lun Zhang,Juanjuan Yin,Kuo Wei,Bingfan Li,Tifeng Jiao,Yan Chen,Jingxin Zhou,Qiuming Peng

The construction of low-cost, high-performance electrocatalysts instead of platinum catalysts is critical to solving the energy crisis. Here, using simple electrospinning and hydrothermal methods, new MoS2 nanosheets on SrTiO3 nanofibers (NFs) and 2D SrTiO3@MoS2 heterostructure NFs are synthesized. In addition, SrTiO3@MoS2 heterostructure NFs are compared with bare SrTiO3 NFs and MoS2 nanosheets. Importantly, the prepared SrTiO3@MoS2 heterostructure shows better hydrogen-evolution reaction performance than other MoS2-based electrocatalysts with an overpotential of 165 mV at 10 mA cm−2, a Tafel slope of 81.41 mV dec−1, and long-term electrochemical durability of 3000 cycles. Therefore, the present work strongly demonstrates the positive synergy between SrTiO3 NFs and layered MoS2, and also provides a strategy for preparing low-cost and high-activity water-decomposition electrocatalysts.

研究领域: 材料科学 · 能源科学
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