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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 (E_a) 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, MoO_x/Ni₃S₂ spheres comprising Ni₃S₂ nanoparticles inside and oxygen-deficient amorphous MoO_x outside in situ grow on Ni foam (NF), to assembly the heterostructure composites of MoO_x/Ni₃S₂/NF. By adjusting volume ratio of the solvents of ethanol to water, the optimized MoO_x/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 MoO_x 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 MoO_x/Ni₃S₂ heterostructure are both beneficial to the reduced Gibbs free energy of hydrogen adsorption (|∆G_H*|) 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 MoO_x/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 (ΔG_H*) 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 Zn_xCd₁₋_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 Zn_0.5Cd_0.5S (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 Zn_xCd_1–_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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Multi-functional layered double hydroxides supported by nanoporous gold toward overall hydrazine splitting

《化学科学与工程前沿（英文）》 2024年第18卷第1期 doi: 10.1007/s11705-023-2373-1

摘要： Layered double hydroxides have demonstrated great potential for the oxygen evolution reaction, which is a crucial half-reaction of overall water splitting. However, it remains challenging to apply layered double hydroxides in other electrochemical reactions with high efficiency and stability. Herein, we report two-dimensional multifunctional layered double hydroxides derived from metal-organic framework sheet precursors supported by nanoporous gold with high porosity, which exhibit appealing performances toward oxygen/hydrogen evolution reactions, hydrazine oxidation reaction, and overall hydrazine splitting. The as-prepared catalyst only requires an overpotential of 233 mV to reach 10 mA·cm^–2 toward oxygen evolution reaction. The overall hydrazine splitting cell only needs a cell voltage of 0.984 V to deliver 10 mA·cm^–2, which is far more superior than that of the overall water splitting system (1.849 V). The appealing performances of the catalyst can be contributed to the synergistic effect between the metal components of the layered double hydroxides and the supporting effect of the nanoporous gold substrate, which could endow the sample with high surface area and excellent conductivity, resulting in superior activity and stability.

关键词： layered double hydroxide oxygen evolution reaction hydrazine oxidation reaction overall hydrazine splitting hydrogen production

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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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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

Multi-functional layered double hydroxides supported by nanoporous gold toward overall hydrazine splitting

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

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