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Polypyrrole@NiCo hybrid nanotube arrays as high performance electrocatalyst for hydrogen evolution reaction

Shenghua Ye, Gaoren Li

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 473-480 doi: 10.1007/s11705-018-1724-9

摘要：

The polypyrrole(PPy)@NiCo hybrid nanotube arrays have been successfully fabricated as a high performance electrocatalyst for hydrogen evolution reaction (HER) in alkaline solution. The strong electronic interactions between PPy and NiCo alloy are confirmed by X-ray photoelectron spectroscopy and Raman spectra. Because these interations can remarkably reduce the apparent activation energy (Ea) for HER and enhance the turnover frequency of catalysts, the electrocatalytic performance of PPy@NiCo hybrid nanotube arrays are significantly improved. The electrochemical tests show that the PPy@NiCo hybrid catalysts exhibit a low overpotential of ~186 mV at 10.0 mA·cm−2 and a small tafel slope of 88.6 mV·deg−1 for HER in the alkaline solution. The PPy@NiCo hybrid nanotubes also exhibit high catalytic activity and high stability for HER.

关键词： NiCo alloy     polypyrrole     hybrid nanotube     electrocatalyst     hydrogen evolution reaction    

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NiS heterostructure grown on nickel foam as efficient and durable self-supported electrocatalysts for hydrogenevolution reaction

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 437-448 doi: 10.1007/s11705-022-2228-1

摘要： High-performance and ultra-durable electrocatalysts are vital for hydrogen evolution reaction (HER) during water splitting. Herein, by one-pot solvothermal method, MoOx/Ni3S2 spheres comprising Ni3S2 nanoparticles inside and oxygen-deficient amorphous MoOx outside in situ grow on Ni foam (NF), to assembly the heterostructure composites of MoOx/Ni3S2/NF. By adjusting volume ratio of the solvents of ethanol to water, the optimized MoOx/Ni3S2/NF-11 exhibits the best HER performance, requiring an extremely low overpotential of 76 mV to achieve the current density of 10 mA∙cm‒2 (η10 = 76 mV) and an ultra-small Tafel slope of 46 mV∙dec‒1 in 0.5 mol∙L‒1 H2SO4. More importantly, the catalyst shows prominent high catalytic stability for HER (> 100 h). The acid-resistant MoOx wraps the inside Ni3S2/NF to ensure the high stability of the catalyst under acidic conditions. Density functional theory calculations confirm that the existing oxygen vacancy and MoOx/Ni3S2 heterostructure are both beneficial to the reduced Gibbs free energy of hydrogen adsorption (|∆GH*|) over Mo sites, which act as main active sites. The heterostructure effectively decreases the formation energy of O vacancy, leading to surface reconstruction of the catalyst, further improving HER performance. The MoOx/Ni3S2/NF is promising to serve as a highly effective and durable electrocatalyst toward HER.

关键词： molybdenum oxides     oxygen vacancies     heterostructure     electrocatalysts     hydrogen evolution reaction    

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Erratum to: Polypyrrole@NiCo hybrid nanotube arrays as high performance electrocatalyst for hydrogenevolution reaction in alkaline solution

Shenghua Ye, Gaoren Li

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 845-845 doi: 10.1007/s11705-019-1879-z

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growth of NiSe nanocrystalline array on graphene for efficient hydrogen evolution reaction

Shuai JI, Changgan LAI, Huan ZHOU, Helin WANG, Ling MA, Cong WANG, Keying ZHANG, Fajun LI, Lixu LEI

《能源前沿（英文）》 2022年 第16卷 第4期   页码 595-600 doi: 10.1007/s11708-022-0827-7

摘要： Nickel selenide electrocatalysts for hydrogen evolution reaction (HER) with a high efficiency and a low-cost have a significant potential in the development of water splitting. However, the inferiority of the high overpotential and poor stability restricts their practical applications. Herein, a composite nanostructure consists of ultrasmall NiSe2 nanocrystals embedded on graphene by microwave reaction is reported. The prepared NiSe2/reduced graphite oxide (rGO) electrocatalyst exhibited a high HER activity with an overpotential of 158 mV at a current density of 10 mA/cm2 and a corresponding moderate Tafel slope of 56 mV/dec in alkaline electrolyte. In addition, a high retention of electrochemical properties (approximately 100%) was demonstrated with an unchangeable microstructure after 100 h of continuous operation.

关键词： nickel selenide     carbon materials     nanoparticles     hydrogen evolution reaction (HER)     microwave reaction    

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An overview and recent advances in electrocatalysts for direct seawater splitting

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1408-1426 doi: 10.1007/s11705-021-2102-6

摘要： In comparison to pure water, seawater is widely accepted as an unlimited resource. The direct seawater splitting is economical and eco-friendly, but the key challenges in seawater, especially the chlorine-related competing reactions at the anode, seriously hamper its practical application. The development of earth-abundant electrocatalysts toward direct seawater splitting has emerged as a promising strategy. Highly efficient electrocatalysts with improved selectivity and stability are of significance in preventing the interference of side reactions and resisting various impurities. This review first discusses the macroscopic understanding of direct seawater electrolysis and then focuses on the strategies for rational design of electrocatalysts toward direct seawater splitting. The perspectives of improved electrocatalysts to solve emerging challenges and further development of direct seawater splitting are also provided.

关键词： seawater splitting     electrocatalysts     oxygen evolution reaction     hydrogen evolution reaction     chlorine chemistry    

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Tuning the electronic structure of NiCoP arrays through V doping for pH-universal hydrogen evolutionreaction electrocatalyst

Yu Lin, Jinlei Wang, Duanlin Cao, Yaqiong Gong

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1134-1146 doi: 10.1007/s11705-020-2014-x

摘要： The exploration of cost-effective, high-performance, and stable electrocatalysts for the hydrogen evolution reaction (HER) over wide pH range (0–14) is of paramount importance for future renewable energy conversion technologies. Regulation of electronic structure through doping vanadium atoms is a feasible construction strategy to enhance catalytic activities, electron transfer capability, and stability of the HER electrode. Herein, V-doped NiCoP nanosheets on carbon fiber paper (CFP) (denoted as V -NiCoP/CFP) were constructed by doping V modulation on NiCoP nanosheets on CFP and used for pH-universal HER. Benefiting from the abundant catalytic sites and optimized hydrogen binding thermodynamics, the resultant V -NiCoP/CFP demonstrates a significantly improved HER catalytic activity, requiring overpotentials of 46.5, 52.4, and 85.3 mV to reach a current density of 10 mA·cm in 1 mol·L KOH, 0.5 mol·L H SO , and 1 mol·L phosphate buffer solution (PBS) electrolytes, respectively. This proposed cation-doping strategy provides a new inspiration to rationally enhance or design new-type nonprecious metal-based, highly efficient, and pH-universal electrocatalysts for various energy conversion systems.

关键词： hydrogen evolution reaction     transition metal phosphides     pH-universal     vanadium doping     carbon fiber paper    

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Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient multifunctional electrocatalysts

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1487-1499 doi: 10.1007/s11705-021-2085-3

摘要： Developing cost-effective electrocatalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is vital in energy conversion and storage applications. Herein, we report a simple method for the synthesis of graphene-reinforced CoS/C nanocomposites and the evaluation of their electrocatalytic performance for typical electrocatalytic reactions. Nanocomposites of CoS embedded in N, S co-doped porous carbon and graphene (CoS@C/Graphene) were generated via simultaneous sulfurization and carbonization of one-pot synthesized graphite oxide-ZIF-67 precursors. The obtained CoS@C/Graphene nanocomposites were characterized by X-ray diffraction, Raman spectroscopy, thermogravimetric analysis-mass spectroscopy, scanning electronic microscopy, transmission electronic microscopy, X-ray photoelectron spectroscopy and gas sorption. It is found that CoS nanoparticles homogenously dispersed in the in situ formed N, S co-doped porous carbon/graphene matrix. The CoS@C/10Graphene composite not only shows excellent electrocatalytic activity toward ORR with high onset potential of 0.89 V, four-electron pathway and superior durability of maintaining 98% of current after continuously running for around 5 h, but also exhibits good performance for OER and HER, due to the improved electrical conductivity, increased catalytic active sites and connectivity between the electrocatalytic active CoS and the carbon matrix. This work offers a new approach for the development of novel multifunctional nanocomposites for the next generation of energy conversion and storage applications.

关键词： MOF derivative     graphene     electrocatalyst     oxygen reduction reaction     oxygen evolution reaction     hydrogen evolution reaction    

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Facile route to achieve MoSe-NiSe on nickel foam as efficient dual functional electrocatalysts for overall water splitting

《能源前沿（英文）》 2022年 第16卷 第3期   页码 483-491 doi: 10.1007/s11708-022-0813-0

摘要： Since the catalytic activity of present nickel-based synthetic selenide is still to be improved, MoSe2-Ni3Se2 was synthesized on nickel foam (NF) (MoSe2-Ni3Se2/NF) by introducing a molybdenum source. After the molybdenum source was introduced, the surface of the catalyst changed from a single-phase structure to a multi-phase structure. The catalyst surface with enriched active sites and the synergistic effect of MoSe2 and Ni3Se2 together enhance the hydrogen evolution reactions (HER), the oxygen evolution reactions (OER), and electrocatalytic total water splitting activity of the catalyst. The overpotential of the MoSe2-Ni3Se2/NF electrocatalyst is only 259 mV and 395 mV at a current density of 100 mA/cm2 for HER and OER, respectively. MoSe2-Ni3Se2/NF with a two-electrode system attains a current density of 10 mA/cm2 at 1.60 V. In addition, the overpotential of HER and OER of MoSe2-Ni3Se2/NF within 80000 s and the decomposition voltage of electrocatalytic total water decomposition hardly changed, showing an extremely strong stability. The improvement of MoSe2-Ni3Se2/NF catalytic activity is attributed to the establishment of the multi-phase structure and the optimized inoculation of the multi-component and multi-interface.

关键词： three-dimensional molybdenum nanomaterials     hydrogen evolution reaction     oxygen evolution reaction     overall water splitting    

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growth of phosphorized ZIF-67-derived amorphous CoP/Cu2O@CF electrocatalyst for efficient hydrogenevolution reaction

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1430-1439 doi: 10.1007/s11705-023-2320-1

摘要： Transition metal phosphides have been extensively studied for catalytic applications in water splitting. Herein, we report an in situ phosphorization of zeolitic imidazole frameworks (ZIF-67) to generate amorphous cobalt phosphide/ZIF-67 heterojunction on a self-supporting copper foam (CF) substrate with excellent performance for hydrogen evolution reaction (HER). The needle-leaf like copper hydroxide was anchored on CF surface, which acted as implantation to grow ZIF-67. The intermediate product was phosphorized to obtain final electrocatalyst (CoP/Cu2O@CF) with uniform particle size, exhibiting a rhombic dodecahedron structure with wrinkles on the surface. The electrochemical measurement proved that CoP/Cu2O@CF catalyst exhibited excellent HER activity and long-term stability in 1.0 mol·L–1 KOH solution. The overpotential was only 62 mV with the Tafel slope of 83 mV·dec–1 at a current density of 10 mA·cm–2, with a large electrochemical active surface area. It also showed competitive performance at large current which indicated the potential application to industrial water electrolysis to produce hydrogen. First-principle calculations illustrated that benefit from the construction of CoP/ZIF-67 heterojunction, the d-band center of CoP downshifted after bonding with ZIF-67 and the Gibbs free energy (ΔGH*) changed from –0.18 to –0.11 eV, confirming both decrease in overpotential and excellent HER activity. This work illustrates the efficient HER activity of CoP/Cu2O@CF catalyst, which will act as a potential candidate for precious metal electrocatalysts.

关键词： CoP/Cu2O@CF     electrocatalyst     phosphorization     HER     DFT    

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Superior performance in visible-light-driven hydrogen evolution reaction of three-dimensionally ordered

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1561-1571 doi: 10.1007/s11705-021-2089-z

摘要： It is of broad interest to develop emerging photocatalysts with excellent light-harvesting capacity and high charge carrier separation efficiency for visible light photocatalytic hydrogen evolution reaction. However, achieving satisfying hydrogen evolution efficiency under noble metal-free conditions remains challenging. In this study, we demonstrate the fabrication of three-dimensionally ordered macroporous SrTiO3 decorated with ZnxCd1−xS nanoparticles for hydrogen production under visible light irradiation (λ>420 nm). Synergetic enhancement of photocatalytic activity is achieved by the slow photon effect and improved separation efficiency of photogenerated charge carriers. The obtained composites could afford very high hydrogen production efficiencies up to 19.67 mmol·g−1·h−1, with an apparent quantum efficiency of 35.9% at 420 nm, which is 4.2 and 23.9 times higher than those of pure Zn0.5Cd0.5S (4.67 mmol·g−1·h−1) and CdS (0.82 mmol·g−1·h−1), respectively. In particular, under Pt-free conditions, an attractive hydrogen production rate (3.23 mmol·g−1·h−1) was achieved, providing a low-cost and high-efficiency strategy to produce hydrogen from water splitting. Moreover, the composites showed excellent stability, and no obvious loss in activity was observed after five cycling tests.

关键词： three-dimensionally ordered macroporous SrTiO3     ZnxCd1–xS     visible light     hydrogen production     promotion mechanism    

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Layered double hydroxide-based core-shell nanoarrays for efficient electrochemical water splitting

Wenfu Xie, Zhenhua Li, Mingfei Shao, Min Wei

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 537-554 doi: 10.1007/s11705-018-1719-6

摘要：

Electrochemical water splitting is an efficient and clean strategy to produce sustainable energy productions (especially hydrogen) from earth-abundant water. Recently, layered double hydroxide (LDH)-based materials have gained increasing attentions as promising electrocatalysts for water splitting. Designing LDHs into hierarchical architectures (e.g., core-shell nanoarrays) is one of the most promising strategies to improve their electrocatalytic performances, owing to the abundant exposure of active sites. This review mainly focuses on recent progress on the synthesis of hierarchical LDH-based core-shell nanoarrays as high performance electrocatalysts for electrochemical water splitting. By classifying different nanostructured materials combined with LDHs, a number of LDH-based core-shell nanoarrays have been developed and their synthesis strategies, structural characters and electrochemical performances are rationally described. Moreover, further developments and challenges in developing promising electrocatalysts based on hierarchical nanostructured LDHs are covered from the viewpoint of fundamental research and practical applications.

关键词： layered double hydroxides (LDHs)     core-shell nanoarrays     oxygen evolution reaction (OER)     hydrogen evolution reaction (HER)     photoelectrochemical water splitting (PEC)    

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High-entropy catalysts for electrochemical water-electrolysis of hydrogen evolution and oxygen evolution

《能源前沿（英文）》 doi: 10.1007/s11708-023-0892-6

摘要： High entropy materials (HEMs) have developed rapidly in the field of electrocatalytic water-electrolysis for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) due to their unique properties. In particular, HEM catalysts are composed of many elements. Therefore, they have rich active sites and enhanced entropy stability relative to single atoms. In this paper, the preparation strategies and applications of HEM catalysts in electrochemical water-electrolysis are reviewed to explore the stabilization of HEMs and their catalytic mechanisms as well as their application in support green hydrogen production. First, the concept and four characteristics of HEMs are introduced based on entropy and composition. Then, synthetic strategies of HEM catalysts are systematically reviewed in terms of the categories of bottom-up and top-down. The application of HEMs as catalysts for electrochemical water-electrolysis in recent years is emphatically discussed, and the mechanisms of improving the performance of electrocatalysis is expounded by combining theoretical calculation technology and ex-situ/in situ characterization experiments. Finally, the application prospect of HEMs is proposed to conquer the challenges in HEM catalyst fabrications and applications.

关键词： high-entropy     electrocatalysis     synthetic methods     water-electrolysis     hydrogen and oxygen evolutions    

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Interface engineering for enhancing electrocatalytic oxygen evolution reaction of CoS/CeO heterostructures

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 376-383 doi: 10.1007/s11705-021-2062-x

摘要： To realize renewable energy conversion, it is important to develop low-cost and high-efficiency electrocatalyst for oxygen evolution reaction. In this communication, a novel bijunction CoS/CeO2 electrocatalyst grown on carbon cloth is prepared by the interface engineering. The interface engineering of CoS and CeO2 facilitates a rapid charge transfer from CeO2 to CoS. Such an electrocatalyst exhibits outstanding electrocatalytic activity with a low overpotential of 311 mV at 10 mA∙cm−2 and low Tafel slope of 76.2 mV∙dec–1, and is superior to that of CoS (372 mV) and CeO2 (530 mV) counterparts. And it has long-term durability under alkaline media.

关键词： interface engineering     CoS/CeO2     electrodeposition     electrocatalyst     oxygen evolution reaction    

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Z-scheme CdS/WO on a carbon cloth enabling effective hydrogen evolution

《能源前沿（英文）》 2021年 第15卷 第3期   页码 678-686 doi: 10.1007/s11708-021-0768-6

摘要： Photocatalytic water splitting for hydrogen (H2) generation is a potential strategy to solve the problem of energy crisis and environmental deterioration. However, powder-like photocatalysts are difficult to recycle, and the agglomeration of particles would affect the photocatalytic activity. Herein, a direct Z-scheme CdS/WO3 composite photocatalyst was fabricated based on carbon cloth through a two-step process. With the support of carbon cloth, photocatalysts tend to grow uniformly for further applications. The experimental results showed that the H2 yield of adding one piece of CdS/WO3 composite material was 17.28 μmol/h, which was 5.5 times as compared to that of pure CdS-loaded carbon cloth material. A cycle experiment was conducted to verify the stability of the as-prepared material and the result demonstrated that the H2 generation performance of CdS/WO3 decreased slightly after 3 cycles. This work provides new ideas for the development of recyclable photocatalysts and has a positive significance for practical applications.

关键词： photocatalysis     CdS/WO3     carbon cloth     Z-scheme     hydrogen evolution    

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Synergistic effect of V and Fe in Ni/Fe/V ternary layered double hydroxides for efficient and durable oxygen evolutionreaction

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 102-115 doi: 10.1007/s11705-022-2179-6

摘要： High-performance and stable electrocatalysts are vital for the oxygen evolution reaction (OER). Herein, via a one-pot hydrothermal method, Ni/Fe/V ternary layered double hydroxides (NiFeV-LDH) derived from Ni foam are fabricated to work as highly active and durable electrocatalysts for OER. By changing the feeding ratio of Fe and V salts, the prepared ternary hydroxides were optimized. At an Fe:V ratio of 0.5:0.5, NiFeV-LDH exhibits outstanding OER activity superior to that of the binary hydroxides, requiring overpotentials of 269 and 274 mV at 50 mA·cm–2 in the linear sweep voltammetry and sampled current voltammetry measurements, respectively. Importantly, NiFeV-LDH shows extraordinary long-term stability (≥ 75 h) at an extremely high current density of 200 mA·cm–2. In contrast, the binary hydroxides present quick decay at 200 mA·cm–2 or even reduced current densities (150 and 100 mA·cm–2). The outstanding OER performance of NiFeV-LDH benefits from the synergistic effect of V and Fe while doping the third metal into bimetallic hydroxide layers: (a) Fe plays a crucial role as the active site; (b) electron-withdrawing V stabilizes the high valence state of Fe, thus accelerating the OER process; (c) V further offers great stabilization for the formed intermediate of FeOOH, thus achieving superior durability.

关键词： oxygen evolution reaction     electrocatalysts     ternary layered double hydroxides     long-term stability    

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标题 作者 时间 类型 操作

Polypyrrole@NiCo hybrid nanotube arrays as high performance electrocatalyst for hydrogen evolution reaction

Shenghua Ye, Gaoren Li

期刊论文

NiS heterostructure grown on nickel foam as efficient and durable self-supported electrocatalysts for hydrogenevolution reaction

期刊论文

Erratum to: Polypyrrole@NiCo hybrid nanotube arrays as high performance electrocatalyst for hydrogenevolution reaction in alkaline solution

Shenghua Ye, Gaoren Li

期刊论文

growth of NiSe nanocrystalline array on graphene for efficient hydrogen evolution reaction

Shuai JI, Changgan LAI, Huan ZHOU, Helin WANG, Ling MA, Cong WANG, Keying ZHANG, Fajun LI, Lixu LEI

期刊论文

An overview and recent advances in electrocatalysts for direct seawater splitting

期刊论文

Tuning the electronic structure of NiCoP arrays through V doping for pH-universal hydrogen evolutionreaction electrocatalyst

Yu Lin, Jinlei Wang, Duanlin Cao, Yaqiong Gong

期刊论文

Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient multifunctional electrocatalysts

期刊论文

Facile route to achieve MoSe-NiSe on nickel foam as efficient dual functional electrocatalysts for overall water splitting

期刊论文

growth of phosphorized ZIF-67-derived amorphous CoP/Cu2O@CF electrocatalyst for efficient hydrogenevolution reaction

期刊论文

Superior performance in visible-light-driven hydrogen evolution reaction of three-dimensionally ordered

期刊论文

Layered double hydroxide-based core-shell nanoarrays for efficient electrochemical water splitting

Wenfu Xie, Zhenhua Li, Mingfei Shao, Min Wei

期刊论文

High-entropy catalysts for electrochemical water-electrolysis of hydrogen evolution and oxygen evolution

期刊论文

Interface engineering for enhancing electrocatalytic oxygen evolution reaction of CoS/CeO heterostructures

期刊论文

Z-scheme CdS/WO on a carbon cloth enabling effective hydrogen evolution

期刊论文

Synergistic effect of V and Fe in Ni/Fe/V ternary layered double hydroxides for efficient and durable oxygen evolutionreaction

期刊论文