ChemCatChem
·
2020
·Vol. 12
·期 11
·3068-3075
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IF 4.853
Ruiqi Zhang,Huixiang Liu,Chenfeng Wang,Lincai Wang,Yanjing Yang,Yanhui Guo
Graphical Hydrogen evolution reaction : A strategy of electroless plating of transition metal boride with high boron content to fabricate binder-free catalytic electrode with superior HER activity has been realized. Facile deposition of transition metal boride (TMB) with high-boron content as highly efficient hydrogen evolution reaction (HER) electrocatalyst has been realized by a facile one-step electroless-plating (EP) method. Boron content of the TMB catalyst shows an appreciable impact on its intrinsic HER activity. NiB/NF electrode with thin amorphous nickel boride (NiB) deposition on nickel foam (NF) required overpotential of only 41.2 mV to deliver a current density of 10 mA cm −2 for HER in 1.0 M KOH alkaline electrolyte. Meanwhile, this kind of electrode also shows satisfied stability which can work at large current density of 1000 mA cm −2 for over 72 h without performance degradation. The advance on the TMB electrode may pave a way to the development of practical electrodes for water splitting.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2021
·
IF 4.094
Yinggang Liu,Shuai Liu,Hanxiao Li,Lijun Yu,Lan Sun,Jiale Xue,Ruojun Xu,Guoxiang Chen
Transition metal dichalcogenides (TMDCs) are considered as the potential electrocatalysts for hydrogen evolution reaction (HER) owing to the two-dimensional (2D) geometry and tunable band gap. However, both the inefficient electron transferring and high Gibbs free energies for hydrogen adsorption (ΔG H *) in MoSe 2 limit its further improvement in catalytic performance. Herein, the few-layered 1T@2H–MoSe 2 composite nanosheets are synthesized by one-pot hydrothermal reaction . It is found that the morphology and composites of nanosheets could be influenced by hydrothermal reaction parameters. As compared to pure 2H–MoSe 2 , 1T@2H–MoSe 2 electrode exhibits remarkable activity for HER with a low overpotential (118 mV), small Tafel slope (65.8 mV·dec −1 ) as well as large electrochemical active area (C dl = 37.5 mF cm −2 ) in acid electrolytes. Density functional theory (DFT) calculations demonstrate that ΔG H * of 1T@2H–MoSe 2 (0.232 eV) is much lower than these of pure 1T-MoSe 2 and 2H–MoSe 2 . It could be ascribed to both the optimized charge transfer and increased density of active sites in 1T@2H–MoSe 2 nanosheets.
研究领域:
材料科学
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电化学
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DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Qingtao Wang,Liqiu Huang,Huiping Liu,Yanxia Wu,Guofu Ma,Ziqiang Lei,Shufang Ren
As a sustainable and green technology for producing high-purity hydrogen, hydrogen evolution reaction (HER) has received extensive attention. The development of an electrocatalyst with good HER activity is the key to economic water electrolysis. Here, this work reports a defect-mediated successive ion layer adsorption and reaction method to construct Ag 2 S/irradiated Sb 2 Te 3 heterojunctions with good HER activity. First, ion irradiation is used to introduce a large number of defects into Sb 2 Te 3 . The defective Sb 2 Te 3 is continuously cyclically immersed in AgNO 3 solution and Na 2 S solution. Ag + and S 2- ions are adsorbed on the defect sites of Sb 2 Te 3 and deposited as Ag 2 S and the heterojunction of Ag 2 S/irradiated Sb 2 Te 3 is obtained. By this strategy, the electrochemical active surface area of the material is increased, reduces the charge transfer resistance, and improves the hydrophilicity of the material surface, thus exhibiting good HER activity. In this work, ion irradiation is used to regulate the surface defects of materials and then to regulate the growth of heterojunction to achieve the purpose of regulating the properties of material. The heterojunction growth method controlled by defect engineering can be widely used in the preparation of heterojunction materials in other energy and environmental fields.
研究领域:
材料科学
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电催化
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能源转换
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DOI
高影响因子
Small Methods
·
2023
·
IF 12.4
Hao Lin,Yang Xu,Xiao Chen,Zengxian Fang,Tian Yan,Kaijie Ma,Le Liu,Jingyu Xi
Vanadium flow batteries (VFBs) face a challenge with the low reaction rates of the V(II)/V(III) redox couple, which limits the performance of VFBs. Additionally, the negative electrode in VFBs is often accompanied by the persistent hydrogen evolution reaction (HER), which is difficult to eliminate. Therefore, understanding the spatial distribution of activity on the negative electrode and the HER side reaction on the electrode surface is of critical importance. This study proposes a weak measurement imaging method to characterize the spatial distribution of surface activity and HER onset potential on the negative electrode in VFBs). This method enables the visualization and in situ detection of key parameters such as the absolute values of |i pa |, |i pc |, |∆E|, |i pc /i pa |, and the HER onset potential. By comparing three different types of graphite felts with varying activity levels, it validates the feasibility of this method. Furthermore, electrochemical stability tests are conducted to study the electrodes repeatability, uniformity, and durability. This method holds promise in guiding the design of electrodes with enhanced activity, good reversibility, minimized HER side reactions, and uniform distribution.
研究领域:
能源存储
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电化学
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材料科学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Xuanxuan Feng,Minghai Zhu,Yu Zhang,Hangning Wang,Fengxiang Qin
Nanoporous high-entropy alloys (HEAs) are emerging as promising electrocatalysts due to their distinctive properties. Surface engineering is an efficient strategy for the further advancement of hydrogen evolution reaction (HER) electrocatalysts. Herein, a maze-like nanoporous CoCrFeNiAl HEA (NPCCF) with fine ligament sizes of ∼17 nm was fabricated using a selective phase dealloying strategy. Compared with commercial thick-ligament porous nickel foam (NF) and as-spun CoCrFeNiAl ribbon, NPCCF, with its nanoscale ligament 3D porosity, possesses a larger electrochemical surface area and exhibits better HER performance. Afterwards, Ni amorphous/crystalline nanoparticles (Ni NPs) with diameters of ∼100 nm were decorated on the NPCCF via a facile electrodeposition method, resulting in a composite electrocatalyst (NPCCF@Ni) designed to boost the HER process. Electrochemical measurements showed that NPCCF@Ni exhibited a low overpotential of 50 mV at a current density of 10 mA cm–2 for HER in 1.0 M KOH. The excellent catalytic activity is attributed to the large active surface area and fast electron transfer ability of the maze-like 3D nanoporous structure decorated with Ni NPs. Theoretical calculations demonstrated that the Ni atoms modified on the CoCrFe model provided a synergistic effect, altering the electronic structure to optimize the adsorption/desorption energy of adsorbed hydrogen (H*) and reduce the reaction energy barrier of the HER process, resulting in lower Gibbs free energy (ΔGH*). This work explores the advantages of nanoporous HEAs as electrocatalysts and provides insights into the design of HER catalysts with excellent performance through surface modification strategies.
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Longyang Liu,Zichen Wang,Xueyan Zhang,Lijie Luo,Yongjun Chen
Highly active and stable electrocatalysts are highly desired for the hydrogen evolution reaction (HER) in water electrolysis. In this study, a ruthenium-ruthenium phosphide heterojunction (Ru-Ru 2 P) anchored on phosphorus-doped graphene (PCSG) was fabricated via a mild molten salt template method. The graphene was synthesized from discarded coconut shells sourced from Hainan. We found that the heterojunction structure could accelerate electron transfer, while the graphene provided more exposed active sites, significantly enhancing the HER activity of the catalyst. The catalyst prepared at 800 °C with 30 mg of RuCl 3 (Ru-Ru 2 P/2D-PCSG-800) exhibited low HER overpotentials of 31 mV in alkaline and 57 mV in acidic electrolytes at a current density of 10 mA cm −2 , respectively, which were comparable to those of commercial 20 % Pt/C catalyst (36 mV in alkaline and 40 mV in acidic electrolytes). Moreover, the catalyst demonstrated high stability with no significant change in current density after 125 hours of operation. Density functional theory calculations revealed that the Ru-Ru 2 P heterojunction could rearrange charge and modify the Ru d -band center, optimizing the adsorption energy of active *H (|ΔG *H |) and breakage energy of *H-OH bond (ΔG H2O ).
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Wei Xia,Congling Li,Li Zhang,Xuemin Yu,Li Zheng,Rui Liu,Aifeng Lv
The development of highly efficient electrocatalysts is of utmost importance for advancing electrochemical energy conversion technologies. Transition metal sulfide heterostructure electrocatalysts have been widely studied and applied in electrocatalysis due to their highly inherent activity in the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) at the interface. We prepared NiS 2 /CoS 2 nanoparticle heterostructures doped with nitrogen-carbon nanotubes (CoS 2 /NiS 2 @N-CNTs) to induce the formation of bifunctional reaction sites. This design contributes to the excellent catalytic activity for electrocatalytic water splitting. The CoS 2 /NiS 2 @N-CNTs electrocatalyst exhibits prominent catalytic activities toward HER and OER, which required low overpotentials of 126 and 205 mV to yield the current density of 10 mA cm −2 in 1 M KOH. The prepared electrocatalysts exhibit fast reaction kinetics with tafel slopes of 71 and 82 mV dec −1 in HER and OER, respectively. The catalyst has a larger electrochemically active surface area (ECSA) of 1030 cm −2 and a strong electron transfer capability with an electrochemical impedance of 41 Ω. These properties are mainly attributed to the unique heterogeneous structure of the catalyst. In addition, CoS 2 /NiS 2 @N-CNTs catalyst is used as both the cathode and anode to fabricate a two-electrode system in a 1.0 M KOH solution measured at 1.53 V. Meanwhile, the stability measurement maintains for 23 h at a current density of 10 mA cm −2 with negligible degradation. This work has successfully developed an approach for rational design and novel synthesis of metal sulfide hybrids as bifunctional electrocatalysts with high activity and stability for overall water splitting.
研究领域:
材料科学
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电化学
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能源技术
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Yuanliang Yuan,Yisheng Yang,Hongxuan Xie,Xiaocong Zhong,Ruixiang Wang,Zhifeng Xu
Due to their distinctive electronic configuration, transition metal phosphides (TMPs) display remarkable catalytic ability in both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER). Several strategies have been proposed to increase the catalytic efficiency of TMPs, including heteroatom doping, morphology design, and interface engineering. In this study, CoP hollow nanoflower clusters doped with trace amounts of Fe (Fe–CoP nanoFC) were synthesized via a template-based hydrothermal reaction and high-temperature phosphatization. Compared with those of Fe 2 P and CoP, the OER and HER overpotentials (@10 mA cm −2 ) of the Fe–CoP nanoFC in alkaline solution (pH = 14) were 269 mV and 203 mV, respectively, outperforming those of commercial RuO 2 (326 mV) and 20% Pt/C (221 mV). The overall water electrolysis voltage with the Fe–CoP nanoFC as both HER and OER catalysts was 1.671 V (@10 mA cm −2 ), outperforming the 1.736 V achieved with commercialized Pt/C || RuO 2 . Furthermore, the voltage remained stable during the 14 h of galvanostatic water electrolysis, indicating the potential for long-term stability. Trace Fe doping facilitates the construction of abundant Fe 2 P/CoP heterojunctions, effectively modulates the charge distribution at the interface, and consequently enhances the OER/HER catalytic efficiency of CoP nanoFCs. DFT calculations indicate that the CoP/Fe 2 P heterojunction interface has a higher d-band center and greater local charge density. These properties increase the adsorption strength of OH∗, O∗ and OOH∗, reduce the free energy of adsorption of hydrogen atoms and improve the stability of H∗. As a result, the catalysts exhibit considerable catalytic capacity for the OER and HER.
研究领域:
材料科学
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催化化学
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能源科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Xuzhuo Sun,Xuyun Gao,Jing Chen,Xin Wang,Haixia Chang,Bo Li,Dengmeng Song,Jun Li,Haisheng Li,Ning Wang
Nanostructuring and metal–support interactions have been explored as effective methods to improve the electrocatalytic activity in heterogeneous catalysis. In this study, we have fabricated ultrasmall Ru nanoparticles (NPs) dispersed on S-doped graphene (denoted as Ru/S-rGO) by a facile “one-pot” procedure. The experimental results indicated that both the S doping and moderate degree of oxidization of GO can induce the formation and high dispersion of the ultrasmall Ru NPs with larger electrochemically active surface areas for exposing more active sites. Metal–support interaction between S-doped graphene and Ru NPs was observed from the X-ray photoelectron spectroscopy and electronic charge-difference studies. It resulted in the decrease in the electron density of Ru, which facilitated electron release from H2O and H–OH bond breakage. The results of density functional theory calculation confirmed that the S-dopants could reduce the energy barrier for breaking the H–OH bond to accelerate water dissociation during the alkaline hydrogen evolution reaction (HER). At a current density 20 mA cm–2, the lowest overpotential of 14 mV, superior to that of Pt/C in alkaline solution, was observed for Ru/S-rGO-24. The observed lowest value of overpotential was because of the ultrasmall size, high dispersion, and metal–support interaction. This work provides a simple and effective method in designing advanced electrocatalysts for the HER in an alkaline electrolyte.
研究领域:
材料科学
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电催化
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能源化学
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产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Wenhui Fang,Jing Wang,Ye Hu,Xiaoqing Cui,Ruifeng Zhu,Yuhua Zhang,Chaochao Yue,Jiaqi Dang,Wei Cui,Hong Zhao,Zengxi Li
It's a major challenge to explore highly active and stable electrocatalysts for efficient hydrogen evolution reactions (HER) and oxygen evolution reactions (OER). In this work, we report a new hybrid electrocatalyst: iron-cobalt decorated nitrogen doped carbon/reduced graphene oxide-700 °C (Fe-Co-CN/rGO-700). The catalyst shows an excellent electrocatalytic performance toward HER and OER in alkaline solution, which has lower overpotentials of 0.215 V and 0.308 V at the current density 10 mA cm −2 , respectively, and this catalyst has an outstanding durability (after 45 h). The excellent activity mainly benefit from the highly dispersed iron/cobalt species, sheet structure with high porosity, the improvement of electronic structures with nitrogen-doped carbon and high conductivity of rGO. Combined with the density function theory (DFT) calculations, the improvement of the HER and OER performance were also attributed to the balance of adsorption/desorption of the hydrogen and oxygen-containing intermediates, and the increased electronic states density near the Fermi level. The proposed work provides a novel and simple strategy to synthesize a porous carbon electrocatalyst material using metal-organic frameworks (MOFs) as precursor with high activity and strong stability for HER and OER.
研究领域:
材料科学
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电催化
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DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 25
·14451-14458
·
IF 12.732
Yonggang Liu,Haijing Li,Junfu Li,Xiaoshuang Ma,Zhiming Cui,Daqiang Gao,Zhenghua Tang
Two-dimensional (2D) rhenium disulfide (ReS2) has been attracting immense interest as a highly promising hydrogen evolution reaction (HER) electrocatalyst recently. However, the HER catalytic active sites of ReS2 are still limited to the finite edges of the nanosheets and the basal-plane is catalytically inert. How to activate the in-plane catalytic activity of ReS2 accordingly becomes the sticking point to further boost its H2 evolution efficiency. Here, the fluorinated ReS2 hierarchical structure assembled as ultrathin nanosheets is proved to exhibit excellent HER activity, where the optimal sample of ReS2-F5.93 shows a low overpotential of 142 mV vs. RHE at a current density of 10 mA cm−2, a Tafel slope of 64 mV dec−1, and significantly improved stability. The enhanced HER performance is mainly attributed to the synergistic effects of increased in-plane active sites and remarkably accelerated charge transfer kinetics. The density functional theory calculation results reveal that F doping can yield the optimal H* adsorption Gibbs free energy and meanwhile increase the electronic states near the Fermi level for accelerated electron transfer. This work can broaden the horizon for designing efficient HER electrocatalysts via activating the in-plane catalytic activity of transition metal dichalcogenides (TMDs).
研究领域:
材料科学
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电化学
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理论计算
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Ruge Zhao,Baoxia Ni,Luming Wu,Pingchuan Sun,Tiehong Chen
Efficient catalysts for hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) are of paramount importance for electrochemical energy applications. Herein, a high-efficient carbon-based trifunctional electrocatalyst FeCoP/C is synthesized through a simple one-step supramolecular-assisted method, in which a supramolecular gel structure is formed by phosphoric acid and melamine to allow the efficient and homogeneous incorporation of highly active species. Experimentally, the as-obtained catalysts exhibit practical trifunctional activities in the ORR, OER, and HER. In alkaline electrolytes , requiring overpotentials of 95 and 282 mV to deliver a current density of 10 mA cm −2 for HER and OER, respectively, and presents the significantly increased alkalic ORR activity, with the half-wave potential of 0.849 V. Furthermore, the FeCoP/C also showed good integrated capabilities for Zn-air batteries. This supramolecular-assisted strategy could bring new inspiration to boost the electrocatalytic performance of transition metal-based electrocatalysts for energy conversion applications.
研究领域:
材料科学
·
电化学
·
能源转换
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）