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>In situ growth of phosphorized ZIF-67-derived amorphous CoP/Cu2O@CF electrocatalyst

《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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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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Erratum to: Polypyrrole@NiCo hybrid nanotube arrays as high performance electrocatalyst for hydrogen

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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NiFeRuOx nanosheets on Ni foam as an electrocatalyst for efficient

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1698-1706 doi: 10.1007/s11705-023-2334-8

摘要： The electrocatalyst NiFeRuOx/NF, comprised of NiFeRuOx nanosheets grown on Ni foam, was synthesized using a hydrothermal process followed by thermal annealing. NiFeRuOx/NF displays high electrocatalytic activity and stability for overall alkaline seawater splitting: 98 mV@ 10 mA∙cm−2 in hydrogen evolution reaction, 318 mV@ 50 mA∙cm−2 in oxygen evolution reaction, and a cell voltage of 1.53 V@ 10 mA∙cm−2, as well as 20 h of durability. A solar-driven system containing such a bifunctional NiFeRuOx/NF has an almost 100% Faradaic efficiency. The NiFeRuOx coating around Ni foam is an anti-corrosion layer and also a critical factor for enhancement of bifunctional performances.

关键词： NiFeRuOx nanosheets     Ni foam     electrocatalysis     overall seawater splitting     solar-driven system    

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Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional electrocatalyst

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1707-1717 doi: 10.1007/s11705-023-2308-x

摘要： Water electrolysis technology is considered to be one of the most promising means to produce hydrogen. Herein, aiming at the problems of high overpotential and slow kinetics in water splitting, N-doped porous carbon nanofibers-coupled CoNi2S4 nanoparticles are prepared as bifunctional electrocatalyst. In the strategy, NaCl is used as the template to prepare porous carbon nanofibers with a large surface area, and sulfur vacancies are created to modulate the electronic structure of CoNi2S4. Electron spin resonance confirms the formation of abundant sulfur vacancies, which largely reduce the bandgap of CoNi2S4 from 1.68 to 0.52 eV. The narrowed bandgap is conducive to the migration of valence electrons and decreases the charge transfer resistance for electrocatalytic reaction. Moreover, the uniform distribution of CoNi2S4 nanoparticles on carbon nanofibers can prevent the aggregation and facilitate the exposure of electrochemical active sites. Therefore, the composite catalyst exhibits low overpotentials of 340 mV@100 mA·cm–2 for oxygen evolution reaction and 380 mV@100 mA·cm–2 for hydrogen evolution reaction. The assembled electrolyzer requires 1.64 V to achieve 10 mA·cm–2 for overall water-splitting with good long-term stability. The excellent performance results from the synergistic effect of porous structures, sulfur deficiency, nitrogen doping, and the well-dispersed active component.

关键词： nanoparticle     sulfur vacancy     porous carbon nanofiber     transition metal sulfides     electrolysis    

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nanostructured NiCoP nanosheets supported on N-doped carbon coated Ni foam as a highly active bifunctional electrocatalyst

Miaomiao Tong, Lei Wang, Peng Yu, Xu Liu, Honggang Fu

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 417-424 doi: 10.1007/s11705-018-1711-1

摘要：

A highly active bi-functional electrocatalyst towards both hydrogen and oxygen evolution reactions is critical for the water splitting. Herein, a self-supported electrode composed of 3D network nanostructured NiCoP nanosheets grown on N-doped carbon coated Ni foam (NiCoP/NF@NC) has been synthesized by a hydrothermal route and a subsequent phosphorization process. As a bifunctional electrocatalyst, the NiCoP/NF@NC electrode needs overpotentials of 31.8 mV for hydrogen evolution reaction and 308.2 mV for oxygen evolution reaction to achieve the current density of 10 mA·cm−2 in 1 mol·L−1 KOH electrolyte. This is much better than the corresponding monometal catalysts of CoP/NF@NC and NiP/NF@NC owing to the synergistic effect. NiCoP/NF@NC also exhibits low Tafel slope, and excellent long-term stability, which are comparable to the commercial noble catalysts of Pt/C and RuO2.

关键词： bimetallic phosphides     N-doped carbon     self-support     hydrogen evolution     oxygen evolution    

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Nickel-carbonate nanowire array: An efficient and durable electrocatalyst for water oxidation under nearly

Yuyao Ji, Min Ma, Xuqiang Ji, Xiaoli Xiong, Xuping Sun

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 467-472 doi: 10.1007/s11705-018-1717-8

摘要：

It is highly attractive but still remains a great challenge to develop an efficient electrocatalyst for oxygen evolution reaction under nearly neutral conditions. In this work, we report the transformation of Ni3S2 nanowire array on nickel foam into the amorphous nickel carbonate nanowire array on nickel foam (NiCO3/NF). The resulting NiCO3/NF shows high electrocatalytic activity towards water oxidation and affords current density of 50 mA·cm−2 at overpotential of 395 mV in 1.0 mol·L−1 KHCO3. Moreover, this NiCO3/NF is also durable with a long-term electrochemical durability of 60 h. This catalyst electrode achieves a high turnover frequency of 0.21 mol O2·s−1 at the overpotential of 500 mV.

关键词： water oxidation     NiCO3/NF     nearly neutral conditions     superior activity     electocatalyst    

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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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Copper nanoparticles/polyaniline-derived mesoporous carbon electrocatalysts for hydrazine oxidation

Tao Zhang, Tewodros Asefa

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 329-338 doi: 10.1007/s11705-018-1741-8

摘要：

Copper nanoparticles-decorated polyaniline-derived mesoporous carbon that can serve as noble metal-free electrocatalyst for the hydrazine oxidation reaction (HzOR) is synthesized via a facile synthetic route. The material exhibits excellent electrocatalytic activity toward HzOR with low overpotential and high current density. The material also remains stable during the electrocatalytic reaction for long time. Its good electrocatalytic performance makes this material a promising alternative to conventional noble metal-based catalysts (e.g., Pt) that are commonly used in HzOR-based fuel cells.

关键词： copper nanoparticles     mesoporous carbon     noble metal-free electrocatalyst     hydrazine oxidation reaction     polyaniline    

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Platinum on nitrogen doped graphene and tungsten carbide supports for ammonia electro-oxidation reaction

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 930-938 doi: 10.1007/s11705-021-2130-2

摘要： Ammonia electrooxidation reaction involving multistep electron-proton transfer is a significant reaction for fuel cells, hydrogen production and understanding nitrogen cycle. Platinum has been established as the best electrocatalyst for ammonia oxidation in aqueous alkaline media. In this study, Pt/nitrogen-doped graphene (NDG) and Pt/tungsten monocarbide (WC)/NDG are synthesized by a wet chemistry method and their ammonia oxidation activities are compared to commercial Pt/C. Pt/NDG exhibits a specific activity of 0.472 mA∙cm–2, which is 44% higher than commercial Pt/C, thus establishing NDG as a more effective support than carbon black. Moreover, it is demonstrated that WC as a support also impacts the activity with further 30% increase in comparison to NDG. Surface modification with Ir resulted in the best electrocatalytic activity with Pt-Ir/WC/NDG having almost thrice the current density of commercial Pt/C. This work adds insights regarding the role of NDG and WC as efficient supports along with significant impact of Ir surface modification.

关键词： Ammonia electro-oxidation reaction     electrocatalyst supports     platinum     nitrogen doped graphene     tungsten carbide    

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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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质子交换膜燃料电池的研究进展

任学佑

《中国工程科学》 2005年 第7卷 第1期   页码 86-94

摘要：

论述了质子交换膜燃料电池的开发现状及国内外研究进展；同时介绍了趋于成熟的贮氢技术，包括质子交换膜、双极板、膜电极和电催化剂在内的关键技术、应用以及未来展望。

关键词： 燃料电池     质子交换膜     双极板     膜电极     电催化剂     开发现状    

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Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reduction and oxygen evolution reaction: a density functional theory study

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 570-580 doi: 10.1007/s11705-022-2247-y

摘要： Recently, metal–organic frameworks are one of the potential catalytic materials for electrocatalytic applications. The oxygen reduction reaction and oxygen evolution reaction catalytic activities of heterometallic cluster-based organic frameworks are investigated using density functional theory. Firstly, the catalytic activities of heterometallic clusters are investigated. Among all heterometallic clusters, Fe2Mn–Mn has a minimum overpotential of 0.35 V for oxygen reduction reaction, and Fe2Co–Co possesses the smallest overpotential of 0.32 V for oxygen evolution reaction, respectively 100 and 50 mV lower than those of Pt(111) and RuO2(110) catalysts. The analysis of the potential gap of Fe2M clusters indicates that Fe2Mn, Fe2Co, and Fe2Ni clusters possess good bifunctional catalytic activity. Additionally, the catalytic activity of Fe2Mn and Fe2Co connected through 3,3′,5,5′-azobenzenetetracarboxylate linker to form Fe2M–PCN–Fe2M is explored. Compared with Fe2Mn–PCN–Fe2Mn, Fe2Co–PCN–Fe2Co, and isolated Fe2M clusters, the mixed-metal Fe2Co–PCN–Fe2Mn possesses excellent bifunctional catalytic activity, and the values of potential gap on the Mn and Co sites of Fe2Co–PCN–Fe2Mn are 0.69 and 0.70 V, respectively. Furthermore, the analysis of the electron structure indicates that constructing a mixed-metal cluster can efficiently enhance the electronic properties of the catalyst. In conclusion, the mixed-metal cluster strategy provides a new approach to further design and synthesize high-efficiency bifunctional electrocatalysts.

关键词： bimetallic metal–organic frameworks     bifunctional electrocatalyst     density functional theory     oxygen reduction reaction     oxygen evolution reaction    

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Synthesis of cobalt vanadium nanomaterials for efficient electrocatalysis of oxygen evolution

Meifeng Hao, Mingshu Xiao, Lihong Qian, Yuqing Miao

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 409-416 doi: 10.1007/s11705-017-1689-0

摘要：

A low-cost and high-activity catalyst for oxygen evolution reaction (OER) is the key to the water splitting technology for hydrogen generation. Here we report the use of three solvents, DMF, ethanol and glycol, in the solvothermal synthesis of three nano-catalysts, Co3(VO4)2-I, Co3(VO4)2-II, and Co3(VO4)2-III, respectively. Transmission electron microscope shows Co3(VO4)2-I, II, and III exist as ultrafine nanosheets, ultrathin nanofilms, and ultrafine nanosheet-comprised microspheres, respectively. These Co3(VO4)2 catalysts exhibit OER electrocatalysis, among which the Co3(VO4)2-II shows the lowest onset overpotential of 310 mV and only requires a small overpotential of 330 mV to drive current density of 10 mA/cm2. Due to their high surface free energy, the ultrathin nanofilms of Co3(VO4)2-II exhibits a good immobilization effect with the high electrocatalytic activity for OER.

关键词： Co3(VO4)2     oxygen evolution reaction     electrocatalyst     water splitting    

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Ionic liquid modified Pt/C electrocatalysts for cathode application in proton exchange membrane fuel cells

Huixin Zhang, Jinying Liang, Bangwang Xia, Yang Li, Shangfeng Du

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 695-701 doi: 10.1007/s11705-019-1838-8

摘要： The modification of Pt/C catalyst by using ionic liquids to improve their catalyst activities has been reported by many researchers, but their practical behavior in operating fuel cells is still unknown. In this work, we study the ionic liquid modified Pt/C nanoparticle catalysts within cathodes for proton exchange membrane fuel cells. The influence of the ionic liquid amount, adsorption times and dispersing solvents are investigated. The experiment results show the best performance enhancement is achieved through two-time surface modification with 2 wt-% ionic liquid solution. The mechanisms are explored with the attribution to the high oxygen solubility in the ionic liquid enabling an improved oxygen diffusion in micropores and to good hydrophobicity facilitating water expelling from the active sites in fuel cell operation.

关键词： ionic liquid     PEMFC     electrode     oxygen reduction reaction     electrocatalyst     adsorption    

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标题 作者 时间 类型 操作

>In situ growth of phosphorized ZIF-67-derived amorphous CoP/Cu2O@CF electrocatalyst

期刊论文

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

Shenghua Ye, Gaoren Li

期刊论文

Erratum to: Polypyrrole@NiCo hybrid nanotube arrays as high performance electrocatalyst for hydrogen

Shenghua Ye, Gaoren Li

期刊论文

NiFeRuOx nanosheets on Ni foam as an electrocatalyst for efficient

期刊论文

Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional electrocatalyst

期刊论文

nanostructured NiCoP nanosheets supported on N-doped carbon coated Ni foam as a highly active bifunctional electrocatalyst

Miaomiao Tong, Lei Wang, Peng Yu, Xu Liu, Honggang Fu

期刊论文

Nickel-carbonate nanowire array: An efficient and durable electrocatalyst for water oxidation under nearly

Yuyao Ji, Min Ma, Xuqiang Ji, Xiaoli Xiong, Xuping Sun

期刊论文

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

期刊论文

Copper nanoparticles/polyaniline-derived mesoporous carbon electrocatalysts for hydrazine oxidation

Tao Zhang, Tewodros Asefa

期刊论文

Platinum on nitrogen doped graphene and tungsten carbide supports for ammonia electro-oxidation reaction

期刊论文

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

期刊论文

质子交换膜燃料电池的研究进展

任学佑

期刊论文

Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reduction and oxygen evolution reaction: a density functional theory study

期刊论文

Synthesis of cobalt vanadium nanomaterials for efficient electrocatalysis of oxygen evolution

Meifeng Hao, Mingshu Xiao, Lihong Qian, Yuqing Miao

期刊论文

Ionic liquid modified Pt/C electrocatalysts for cathode application in proton exchange membrane fuel cells

Huixin Zhang, Jinying Liang, Bangwang Xia, Yang Li, Shangfeng Du

期刊论文