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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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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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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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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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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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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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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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Activated carbon induced oxygen vacancies-engineered nickel ferrite with enhanced conductivity for supercapacitor

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 2088-2100 doi: 10.1007/s11705-023-2352-6

摘要： Activated carbon induced oxygen vacancies-engineered nickel ferrite with enhanced conductivity for supercapacitor application

关键词： nickel ferrite conductivity     carbon oxygen vacancies    

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Impact of oxygen enriched combustion on the performance of a single cylinder diesel engine

K. RAJKUMAR, P. GOVINDARAJAN

《能源前沿（英文）》 2011年 第5卷 第4期   页码 398-403 doi: 10.1007/s11708-011-0157-7

摘要： In the present experiment, a computerized single cylinder diesel engine with a data acquisition system was used to study the effects of oxygen enriched combustion technology (OECT) on the performance characteristics. The use of different levels of oxygen-enriched air was compared with respect to percentage load. Increasing the oxygen content in the air leads to faster burn rates and increases the combustibility at the same stoichiometry (oxygen-to-fuel ratio). These effects have the potential to increase the thermal efficiency and specific power output of a diesel engine. The power increases considerably with oxygen enrichment. In addition, oxygen enrichment can also be considered as a way to reduce the sudden loss in power output when the engine operates in a high load condition. Assessed high combustion temperature from the oxygen enriched combustion leads to high combustion efficiency. OECT reduces the volume of flue gases and reduces the effects of greenhouse effects. Engine tests were conducted in the above said engine for different loads and the following performance characteristics like brake power (BP), specific fuel consumption (SFC), mean effective pressure, brake thermal efficiency, mechanical efficiency, and exhaust gas temperature were studied. The objective of this paper is to address, in a systematic way, the key technical issues associated with applying OECT to single cylinder diesel engines.

关键词： oxygen enriched combustion     exhaust gas temperature     brake power (BP)     specific fuel consumption (SFC)    

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Contributions of adsorption, bioreduction and desorption to uranium immobilization by extracellular polymeric

《环境科学与工程前沿（英文）》 2023年 第17卷 第9期 doi: 10.1007/s11783-023-1707-z

摘要：

● EPS immobilizes U(VI) via adsorption, bioreduction and desorption.

关键词： Adsorption     Bioreduction     Desorption     Kinetics     Isotherm     Uranium    

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ionic silver promote the proliferation of human keratinocytes by inducing the production of reactive oxygen

null

《医学前沿（英文）》 2018年 第12卷 第3期   页码 289-300 doi: 10.1007/s11684-017-0550-7

摘要：

Silver-containing preparations are widely used in the management of skin wounds, but the effects of silver ions on skin wound healing remain poorly understood. This study investigated the effects of silver ions (Ag+) on the proliferation of human skin keratinocytes (HaCaT) and the production of intracellular reactive oxygen species (ROS). After treating HaCaT cells with Ag+and/or the active oxygen scavenger N-acetyl cysteine (NAC), cell proliferation and intracellular ROS generation were assessed using CCK-8 reagent and DCFH-DA fluorescent probe, respectively. In addition, 5-bromo-2-deoxyUridine (BrdU) incorporation assays, cell cycle flow cytometry, and proliferating cell nuclear antigen (PCNA) immunocytochemistry were conducted to further evaluate the effects of sub-cytotoxic Ag+ concentrations on HaCaT cells. The proliferation of HaCaT cells was promoted in the presence of 10−6 and 10−5 mol/L Ag+ at 24, 48, and 72 h. Intracellular ROS generation also significantly increased for 5–60 min after exposure to Ag+. The number of BrdU-positive cells and the presence of PCNA in HaCaT cells increased 48 h after the addition of 10−6 and 10−5 mol/L Ag+, with 10−5 mol/L Ag+ markedly increasing the cell proliferation index. These effects of sub-cytotoxic Ag+ concentrations were repressed by 5 mmol/L NAC. Our results suggest that sub-cytotoxic Ag+ concentrations promote the proliferation of human keratinocytes and might be associated with a moderate increase in intracellular ROS levels. This study provides important experimental evidence for developing novel silver-based wound agents or dressings with few or no cytotoxicity.

关键词： ionic silver     human keratinocyte     cell proliferation     reactive oxygen species     active oxygen scavenger     NAC    

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

《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

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

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

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

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

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

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

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

期刊论文

Activated carbon induced oxygen vacancies-engineered nickel ferrite with enhanced conductivity for supercapacitor

期刊论文

Impact of oxygen enriched combustion on the performance of a single cylinder diesel engine

K. RAJKUMAR, P. GOVINDARAJAN

期刊论文

Contributions of adsorption, bioreduction and desorption to uranium immobilization by extracellular polymeric

期刊论文

ionic silver promote the proliferation of human keratinocytes by inducing the production of reactive oxygen

null

期刊论文

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

期刊论文