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Cobalt nanoparticle decorated N-doped carbons derived from a cobalt covalent organic framework for oxygenelectrochemistry

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1550-1560 doi: 10.1007/s11705-021-2104-4

摘要： The low cost and highly efficient construction of electrocatalysts has attracted significant attention owing to the use of clean and sustainable energy technologies. In this work, cobalt nanoparticle decorated N-doped carbons (Co@NC) are synthesized by the pyrolysis of a cobalt covalent organic framework under an inert atmosphere. The Co@NC demonstrates improved electrocatalytic capabilities compared to N-doped carbon without the addition of Co nanoparticles, indicating the important role of cobalt. The well-dispersed active sites (Co-Nx) and the synergistic effect between the carbon matrix and Co nanoparticles greatly enhance the electrocatalytic activity for the oxygen reduction reaction. In addition, the Co content has a significant effect on the catalytic activity. The resulting Co@NC-0.86 exhibits a superb electrocatalytic activity for the oxygen reduction reaction in an alkaline electrolyte in terms of the onset potential (0.90 V), half-wave potential (0.80 V) and the limiting current density (4.84 mA·cm–2), and a high selectivity, as well as a strong methanol tolerance and superior durability, these results are comparable to those of the Pt/C catalyst. Furthermore, the superior bifunctional activity of Co@NC-0.86 was also confirmed in a home-built Zn-air battery, signifying the possibility for application in electrode materials and in current energy conversion and storage devices.

关键词： cobalt embedment     N-doped carbons     covalent organic framework     oxygen reduction     Zn-air battery    

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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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Research progress in tribo-electrochemistry and tribo-electrochemical polishing

ZHAI Wenjie

《机械工程前沿（英文）》 2007年 第2卷 第4期   页码 463-467 doi: 10.1007/s11465-007-0080-0

摘要： In this paper, the status quo and recent progress in the research on tribo-electrochemistry in aqueous and non-aqueous media, respectively, are reviewed. Much more attention has been paid to the tribo-electrochemical mechanisms for the control of friction and wear. Based on a summary of the conventional polishing principles of hard and brittle materials, the tribo-electrochemical polishing method is proposed. The results of the preliminary test show that tribo-electrochemical polishing is promising to become a critical technology in the high efficient polishing and planarization of microelectronic materials.

关键词： tribo-electrochemical mechanisms     planarization     non-aqueous     tribo-electrochemistry     summary    

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Study on tribological and electrochemistry properties of metal materials in H2O2 solutions

Chengqing YUAN, Li YU, Jian LI, Xinping YAN

《机械工程前沿（英文）》 2012年 第7卷 第1期   页码 93-98 doi: 10.1007/s11465-012-0313-8

摘要：

Hydrogen peroxide (H2O2) is a kind of ideal green propellant. It is crucial to study the wear behavior and failure modes of the metal materials under the strong oxidizing environment of H2O2. This study aims to investigate the wear of rubbing pairs of 2Cr13 stainless steel against 1045 metal in H2O2 solutions, which has a great effect on wear, the decomposition and damage mechanism of materials. The comparison analysis of the friction coefficients, wear mass loss, worn surface topographies and current densities was conducted under different concentrations of H2O2 solutions. There were significant differences in the tribological and electrochemistry properties of the rubbing pairs in different H2O2 solutions.

关键词： hydrogen peroxide     wear     corrosion     wear mechanism    

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Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reductionand 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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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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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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A review of Pt-based electrocatalysts for oxygen reduction reaction

Changlin ZHANG, Xiaochen SHEN, Yanbo PAN, Zhenmeng PENG

《能源前沿（英文）》 2017年 第11卷 第3期   页码 268-285 doi: 10.1007/s11708-017-0466-6

摘要： Development of active and durable electrocatalyst for oxygen reduction reaction (ORR) remains one challenge for the polymer electrolyte membrane fuel cell (PEMFC) technology. Pt-based nanomaterials show the greatest promise as electrocatalyst for this reaction among all current catalytic structures. This review focuses on Pt-based ORR catalyst material development and covers the past achievements, current research status and perspectives in this research field. In particular, several important categories of Pt-based catalytic structures and the research advances are summarized. Key factors affecting the catalyst activity and durability are discussed. An outlook of future research direction of ORR catalyst research is provided.

关键词： oxygen reduction reaction (ORR)     electrocatalysis     platinum catalyst     activity     durability    

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Enabling nickel ferrocyanide nanoparticles for high-performance ammonium ion storage

《化学科学与工程前沿（英文）》 2023年 第17卷 第2期   页码 226-235 doi: 10.1007/s11705-022-2198-3

摘要： Prussian blue and its analogs are extensively investigated as a cathode for ammonium-ion batteries. However, they often suffer from poor electronic conductivity. Here, we report a Ni2Fe(CN)6/multiwalled carbon nanotube composite electrode material, which is prepared using a simple coprecipitation approach. The obtained material consists of nanoparticles with sizes 30–50 nm and the multiwalled carbon nanotube embedded in it. The existence of multiwalled carbon nanotube ensures that the Ni2Fe(CN)6/multiwalled carbon nanotube composite shows excellent electrochemical performance, achieving a discharge capacity of 55.1 mAh·g–1 at 1 C and 43.2 mAh·g–1 even at 15 C. An increase in the ammonium-ion diffusion coefficient and ionic/electron conductivity based on kinetic investigations accounts for their high performance. Furthermore, detailed ex situ characterizations demonstrate that Ni2Fe(CN)6/multiwalled carbon nanotube composite offers three advantages: negligible lattice expansion during cycling, stable structure, and the reversible redox couple. Therefore, the Ni2Fe(CN)6/multiwalled carbon nanotube composite presents a long cycling life and high rate capacity. Finally, our study reports a desirable material for ammonium-ion batteries and provides a practical approach for improving the electrochemical performance of Prussian blue and its analogs.

关键词： nickel ferrocyanides     NH4+     electrochemistry     Prussian blue     aqueous ammonium ion batteries    

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Photoreduction adjusted surface oxygen vacancy of BiMoO for boosting photocatalytic redox performance

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1937-1948 doi: 10.1007/s11705-023-2353-5

摘要： In this study, Bi2MoO6 with adjustable rich oxygen vacancies was prepared by a novel and simple solvothermal-photoreduction method which might be suitable for a large-scale production. The experiment results show that Bi2MoO6 with rich oxygen vacancies is an excellent photocatalyst. The photocatalytic ability of BMO-10 is 0.3 and 3.5 times higher than that of the pristine Bi2MoO6 for Rhodamine B degradation and Cr(VI) reduction, respectively. The results display that the band energy of the samples with oxygen vacancies was narrowed and the light absorption was broadened. Meanwhile, the efficiency of photogenerated electron-holes was increased and the separation and transfer speed of photogenerated carriers were improved. Therefore, this work provides a convenient and efficient method to prepare potential adjustable oxygen vacancy based photocatalysts to eliminate the pollution of dyes and Cr(VI) in water.

关键词： Bi2MoO6     oxygen vacancies     photoreduction     Cr(VI)     RhB    

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Role of oxygen vacancy inducer for graphene in graphene-containing anodes

《化学科学与工程前沿（英文）》 2023年 第17卷 第3期   页码 326-333 doi: 10.1007/s11705-022-2213-8

摘要： Currently, graphene is only considered as a conductive additive and expansion inhibitor in oxides/graphene composite anodes. In this study, a new graphene role (oxygen vacancy inducer) in graphene/oxides composites anodes, which are treated at high-temperature, is proposed and verified using experiments and density functional theory calculations. During high-temperature processing, graphene forms carbon vacancies due to increased thermal vibration, and the carbon vacancies capture oxygen atoms, facilitating the formation of oxygen vacancies in oxides. Moreover, the induced oxygen vacancy concentrations can be regulated by sintering temperatures, and the behavior is unaffected by oxide crystal structures (crystalline and amorphous) and morphology (size and shape). According to density functional theory calculations and electrochemical measurements, the oxygen vacancies enhance the lithium-ion storage performance. The findings can result in a better understanding of graphene’s roles in graphene/oxide composite anodes, and provide a new method for designing high-performance oxide anodes.

关键词： oxide     oxygen vacancy     graphene     anode     density functional theory calculation    

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Multivalent manganese oxides with high electrocatalytic activity for oxygen reduction reaction

Xiangfeng Peng, Zhenhai Wang, Zhao Wang, Yunxiang Pan

《化学科学与工程前沿（英文）》 2018年 第12卷 第4期   页码 790-797 doi: 10.1007/s11705-018-1706-y

摘要： A noble-metal-free catalyst based on both Mn O and MnO was prepared by using the dielectric barrier discharge technique at moderate temperature. The prepared catalyst shows a higher electrocatalytic activity towards the oxygen reduction reaction than the catalyst prepared by using the traditional calcination process. The enhanced activity could be due to the coexistence of manganese ions with different valences, the higher oxygen adsorption capacity, and the suppressed aggregation of the catalyst nanoparticles at moderate temperature. The present work would open a new way to prepare low-cost and noble-metal-free catalysts at moderate temperature for more efficient electrocatalysis.

关键词： oxygen reduction reaction     manganese oxides     mixed valences of manganese     oxygen adsorption     dielectric barrier discharge    

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Cooperative effect between copper species and oxygen vacancy in CeZrCuO catalysts for carbon monoxide

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1524-1536 doi: 10.1007/s11705-021-2106-2

摘要： The effects of Zr doping on the existence of Cu and the catalytic performance of Ce0.7−xZrxCu0.3O2 for CO oxidation were investigated. The characterization results showed that all samples have a cubic structure, and a small amount of Zr doping facilitates Cu2+ ions entering the CeO2 lattice, but excessive Zr doping leads to the formation of surface CuO crystals again. Thus, the number of oxygen vacancies caused by the Cu2+ entering the lattice (e.g., Cu2+–□–Ce4+; □: oxygen vacancy), and the amount of reducible copper species caused by CuO crystals, varies with the Zr doping. Catalytic CO oxidation tests indicated that the oxygen vacancy and the reducible copper species were the adsorption and activation sites of O2 and CO, respectively, and the cooperative effects between them accounted for the high CO oxidation activity. Thus, the samples x = 0.1 and 0.3, which possessed the most oxygen vacancy or reducible copper species, showed the best activity for CO oxidation, with full CO conversion obtained at 110 °C. The catalyst is also stable and has good resistance to water during the reaction.

关键词： Ce–Zr–Cu–O     CO oxidation     reducible copper species     oxygen vacancy     cooperative effect    

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Enhanced performance of oxygen vacancies on CO adsorption and activation over different phases of ZrO

《能源前沿（英文）》 2023年 第17卷 第4期   页码 545-554 doi: 10.1007/s11708-023-0867-7

摘要： The effect of oxygen vacancies on the adsorption and activation of CO2 on the surface of different phases of ZrO2 is investigated by density functional theory (DFT) calculations. The calculations show that the oxygen vacancies contribute greatly to both the adsorption and activation of CO2. The adsorption energy of CO2 on the c-ZrO2, t-ZrO2 and, m-ZrO2 surfaces is enhanced to 5, 4, and 3 folds with the help of oxygen vacancies, respectively. Moreover, the energy barrier of CO2 dissociation on the defective surfaces of c-ZrO2, t-ZrO2, and m-ZrO2 is reduced to 1/2, 1/4, and 1/5 of the perfect surface with the assistance of oxygen vacancies. Furthermore, the activation of CO2 on the ZrO2 surface where oxygen vacancies are present, and changes from an endothermic reaction to an exothermic reaction. This finding demonstrates that the presence of oxygen vacancies promotes the activation of CO2 both kinetically and thermodynamically. These results could provide guidance for the high-efficient utilization of CO2 at an atomic scale.

关键词： CO2 activation     oxygen vacancies     ZrO2     different phases    

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Electrochemical CO reduction to C products over CuZn intermetallic catalysts synthesized by electrodeposition

《能源前沿（英文）》 doi: 10.1007/s11708-023-0898-0

摘要： Electrocatalytic CO2 reduction (ECR) offers an attractive approach to realizing carbon neutrality and producing valuable chemicals and fuels using CO2 as the feedstock. However, the lack of cost-effective electrocatalysts with better performances has seriously hindered its application. Herein, a one-step co-electrodeposition method was used to introduce Zn, a metal with weak *CO binding energy, into Cu to form Cu/Zn intermetallic catalysts (Cu/Zn IMCs). It was shown that, using an H-cell, the high Faradaic efficiency of C2+ hydrocarbons/alcohols (FEC2+) could be achieved in ECR by adjusting the surface metal components and the applied potential. In suitable conditions, FEC2+ and current density could be as high as 75% and 40 mA/cm2, respectively. Compared with the Cu catalyst, the Cu/Zn IMCs have a lower interfacial charge transfer resistance and a larger electrochemically active surface area (ECSA), which accelerate the reaction. Moreover, the *CO formed on Zn sites can move to Cu sites due to its weak binding with *CO, and thus enhance the C–C coupling on the Cu surface to form C2+ products.

关键词： carbon dioxide electroreduction     electrochemistry     co-electrodeposition     intermetallic catalysts     value-added chemicals    

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标题 作者 时间 类型 操作

Cobalt nanoparticle decorated N-doped carbons derived from a cobalt covalent organic framework for oxygenelectrochemistry

期刊论文

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

期刊论文

Research progress in tribo-electrochemistry and tribo-electrochemical polishing

ZHAI Wenjie

期刊论文

Study on tribological and electrochemistry properties of metal materials in H2O2 solutions

Chengqing YUAN, Li YU, Jian LI, Xinping YAN

期刊论文

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

期刊论文

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

期刊论文

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

期刊论文

A review of Pt-based electrocatalysts for oxygen reduction reaction

Changlin ZHANG, Xiaochen SHEN, Yanbo PAN, Zhenmeng PENG

期刊论文

Enabling nickel ferrocyanide nanoparticles for high-performance ammonium ion storage

期刊论文

Photoreduction adjusted surface oxygen vacancy of BiMoO for boosting photocatalytic redox performance

期刊论文

Role of oxygen vacancy inducer for graphene in graphene-containing anodes

期刊论文

Multivalent manganese oxides with high electrocatalytic activity for oxygen reduction reaction

Xiangfeng Peng, Zhenhai Wang, Zhao Wang, Yunxiang Pan

期刊论文

Cooperative effect between copper species and oxygen vacancy in CeZrCuO catalysts for carbon monoxide

期刊论文

Enhanced performance of oxygen vacancies on CO adsorption and activation over different phases of ZrO

期刊论文

Electrochemical CO reduction to C products over CuZn intermetallic catalysts synthesized by electrodeposition

期刊论文