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Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctionalelectrocatalyst for overall water splitting

《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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Network nanostructured NiCoP nanosheets supported on N-doped carbon coated Ni foam as a highly active bifunctionalelectrocatalyst for hydrogen and oxygen evolution reactions

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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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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>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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Alkylation of benzene with carbon dioxide to low-carbon aromatic hydrocarbons over bifunctional Zn-Ti

Xiangyu Liu, Yanling Pan, Peng Zhang, Yilin Wang, Guohao Xu, Zhaojie Su, Xuedong Zhu, Fan Yang

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 384-396 doi: 10.1007/s11705-021-2045-y

摘要： Alkylation of benzene to value-added, high octane number and low toxic toluene and xylenes provides a way to lower benzene content in gasoline pool, and is hence a method to promote fuel quality. On the other hand, CO accumulation in the atmosphere causes global warming and requires effective route for its valorization. Utilization of CO as a carbon source for benzene alkylation could achieve both goals. Herein, alkylation of benzene with CO and H was realized by a series of low-cost bifunctional catalysts containing zinc/titanium oxides (Zn/Ti oxides) and HZSM-5 molecular sieves in a fixed-bed reactor. By regulating and controlling oxygen vacancies of Zn/Ti oxides and the acidities of HZSM-5, benzene conversion and CO conversion reached 28.7% and 29.9% respectively, along with a total selectivity of toluene and xylene higher than 90%. In this process, more than 25% CO was effectively utilized and incorporated into the target products. Moreover, the mechanism of the reaction was analyzed and the course was simultaneously traced. CO was transformed into methanol firstly, and then methanol reacted with benzene generating toluene and xylene. The innovation provides a new method for upgrading of fuels and upcycling the emissions of CO , which is of great environmental and economic benefits.

关键词： carbon dioxide     benzene     alkylation     bifunctional catalyst     mechanism    

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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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Metal phosphonate-derived cobalt/nickel phosphide@N-doped carbon hybrids as efficient bifunctional oxygen

《化学科学与工程前沿（英文）》 2022年 第16卷 第9期   页码 1367-1376 doi: 10.1007/s11705-022-2153-3

摘要： The exploration of efficient bifunctional electrocatalysts for oxygen reduction reaction and oxygen evolution reaction is pivotal for the development of rechargeable metal–air batteries. Transition metal phosphides are emerging as promising catalyst candidates because of their superb activity and low cost. Herein, a novel metal phosphonate-derived cobalt/nickel phosphide@N-doped carbon hybrid was developed by a carbothermal reduction of cobalt/nickel phosphonate hybrids with different Co/Ni molar ratios. The metal phosphonate derivation method achieved an intimately coupled interaction between metal phosphides and a heteroatom-doped carbon substrate. The resultant Co2P/Ni3P@NC-0.2 enables an impressive electrocatalytic oxygen reduction reaction activity, comparable with those of state-of-the-art Pt/C catalysts in terms of onset potential (0.88 V), 4e‒ selectivity, methanol tolerance, and long-term durability. Moreover, remarkable oxygen evolution reaction activity was also observed in alkaline conditions. The high activity is ascribed to the N-doping, abundant accessible catalytic active sites, and the synergistic effect among the components. This work not only describes a high-efficiency electrocatalyst for both oxygen reduction reaction and oxygen evolution reaction, but also highlights the application of metal phosphonate hybrids in fabricating metal phosphides with tunable structures, which is of great significance in the energy conversion field.

关键词： metal phosphonate     cobalt/nickel phosphide     N-doped carbon     oxygen electrochemistry     Zn−air battery    

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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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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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用于个人降温和保暖的具有定制热传导和热辐射特性的双功能非对称织物 Article

Yucan Peng, Hiang Kwee Lee, David S. Wu, Yi Cui

《工程（英文）》 2022年 第10卷 第3期   页码 167-173 doi: 10.1016/j.eng.2021.04.016

摘要：

为了让人体感到热舒适，同时节约能源，个人热管理正逐渐成为一种颇有前景的策略。通过更好地控制人体散热，个人热管理可以实现有效的个人降温和保暖。本文提出了一种简单的表面改性方法，在商用织物的基础上定制热传导和热辐射特性，以便更好地管理从人体到环境的整个传热路径。本文对一种同时具有降温和保暖效果的双功能非对称织物（BAF）进行论证。凭借粗糙度不对称和表面改性等优点，BAF在降温模式下通过增强热传导和热辐射表现出显著的降温效果；在保暖模式下，两条路径的散热都减少，从而实现个人保暖。结果表明，在BAF的降温和保暖模式下测得的皮肤温差可达4.6 ℃，表明一件BAF衣服可以扩大人体的热舒适区。希望本研究可为用于个人热管理的织物的设计提供新的视角，并为现有的用于个人降温和保暖的织物的简单改性提供新的解决方案。

关键词： 织物     个人热管理     双功能非对称织物     热传导     热辐射    

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ZnZr/HZSM-5 as efficient catalysts for alkylation of benzene with carbon dioxide

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 404-414 doi: 10.1007/s11705-022-2215-6

摘要： Alkylation of benzene with carbon dioxide and hydrogen to produce toluene and xylene could increase the added-value of surplus benzene as well as relieve environmental problems like green-house effect. In this work, the alkylation benzene with carbon dioxide and hydrogen reaction was proceeded by using the mixture of zinc-zirconium oxide and HZSM-5 as bifunctional catalyst. The equivalent of Zn/Zr = 1 displays the best catalytic performance at 425 °C and 3.0 MPa, and benzene conversion reaches 42.9% with a selectivity of 90% towards toluene and xylene. Moreover, the carbon dioxide conversion achieves 23.3% and the carbon monoxide selectivity is lower than 35%, indicating that more than 50% carbon dioxide has been effectively incorporated into the target product, which is the best result as far as we know. Combined with characterizations, it indicated that the Zn and Zr formed a solid solution under specific conditions (Zn/Zr = 1). The as-formed solid solution not only possesses a high surface area but also provides a large amount of oxygen vacancies. Additionally, the bifunctional catalyst has excellent stabilities that could keep operating without deactivation for at least 80 h. This work provides promising industrial applications for the upgrading of aromatics.

关键词： carbon dioxide     alkylation of benzene     solid solution catalyst     bifunctional catalyst    

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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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标题 作者 时间 类型 操作

Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctionalelectrocatalyst for overall water splitting

期刊论文

Network nanostructured NiCoP nanosheets supported on N-doped carbon coated Ni foam as a highly active bifunctionalelectrocatalyst for hydrogen and oxygen evolution reactions

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

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

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

期刊论文

Alkylation of benzene with carbon dioxide to low-carbon aromatic hydrocarbons over bifunctional Zn-Ti

Xiangyu Liu, Yanling Pan, Peng Zhang, Yilin Wang, Guohao Xu, Zhaojie Su, Xuedong Zhu, Fan Yang

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

Metal phosphonate-derived cobalt/nickel phosphide@N-doped carbon hybrids as efficient bifunctional oxygen

期刊论文

NiFeRuOx nanosheets on Ni foam as an electrocatalyst for efficient

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

用于个人降温和保暖的具有定制热传导和热辐射特性的双功能非对称织物

Yucan Peng, Hiang Kwee Lee, David S. Wu, Yi Cui

期刊论文

ZnZr/HZSM-5 as efficient catalysts for alkylation of benzene with carbon dioxide

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