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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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In situ DRIFTS study of photocatalytic CO 2 reduction under UV irradiation

Jeffrey C. S. WU, Chao-Wei HUANG,

《化学科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 120-126 doi: 10.1007/s11705-009-0232-3

摘要： Photocatalytic reduction of CO on TiO and Cu/TiO photocatalysts was studied by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) under UV irradiation. The photocatalysts were prepared by sol-gel method via controlled hydrolysis of titanium (IV) butoxide. Copper precursor was loaded onto TiO during sol-gel procedure. A large amount of adsorbed HO and surface OH groups was detected at 25°C on the TiO photocatalyst after being treated at 500°C under air stream. Carbonate and bicarbonate were formed rapidly due to the reaction of CO with oxygen-vacancy and OH groups, respectively, on TiO surface upon CO adsorption. The IR spectra indicated that, under UV irradiation, gas-phase CO further combined with oxygen-vacancy and OH groups to produce more carbonate or bicarbonate. The weak signals of reaction intermediates were found on the IR spectra, which were due to the slow photocatalytic CO reduction on photocatalysts. Photogenerated electrons merge with H ions to form H atoms, which progressively reduce CO to form formic acid, dioxymethylene, formaldehyde and methoxy as observed in the IR spectra. The well-dispersed Cu, acting as the active site significantly increases the amount of formaldehyde and dioxymethylene, thus promotes the photoactivity of CO reduction on Cu/TiO. A possible mechanism of the photocatalytic CO reduction is proposed based on these intermediates and products on the photocatalysts.

关键词： irradiation     oxygen-vacancy     Photocatalytic reduction     Carbonate     butoxide    

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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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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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Catalytic oxidation of CO over Pt/Fe

Zihao Li, Yang Geng, Lei Ma, Xiaoyin Chen, Junhua Li, Huazhen Chang, Johannes W. Schwank

《环境科学与工程前沿（英文）》 2020年 第14卷 第4期 doi: 10.1007/s11783-020-1244-y

摘要： Abstract • Strong metal-support interaction exists on Pt/Fe3O4 catalysts. • Pt metal particles facilitate the formation of oxygen vacancies on Fe3O4. • Fe3O4 supports enhance the strength of CO adsorption on Pt metal particles. The self-inhibition behavior due to CO poisoning on Pt metal particles strongly impairs the performance of CO oxidation. It is an effective method to use reducible metal oxides for supporting Pt metal particles to avoid self-inhibition and to improve catalytic performance. In this work, we used in situ reductions of chloroplatinic acid on commercial Fe3O4 powder to prepare heterogeneous-structured Pt/Fe3O4 catalysts in the solution of ethylene glycol. The heterogeneous Pt/Fe3O4 catalysts achieved a better catalytic performance of CO oxidation compared with the Fe3O4 powder. The temperatures of 50% and 90% CO conversion were achieved above 260°C and 290°C at Pt/Fe3O4, respectively. However, they are accomplished on Fe3O4 at temperatures higher than 310°C. XRD, XPS, and H2-TPR results confirmed that the metallic Pt atoms have a strong synergistic interaction with the Fe3O4 supports. TGA results and transient DRIFTS results proved that the Pt metal particles facilitate the release of lattice oxygen and the formation of oxygen vacancies on Fe3O4. The combined results of O2-TPD and DRIFTS indicated that the activation step of oxygen molecules at surface oxygen vacancies could potentially be the rate-determining step of the catalytic CO oxidation at Pt/Fe3O4 catalysts. The reaction pathway involves a Pt-assisted Mars-van Krevelen (MvK) mechanism.

关键词： Strong metal-support interaction (SMSI)     Surface oxygen vacancy     Lattice oxygen     Magnetite     Platinum metals    

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Zinc modification of Ni-Ti as efficient NiZnTi catalysts with both geometric and electronic improvements for hydrogenation of nitroaromatics

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 461-474 doi: 10.1007/s11705-021-2072-8

摘要： The catalytic hydrogenation of nitroaromatics is an environmentally friendly technology for aniline production, and it is crucial to develop noble-metal-free catalysts that can achieve chemoselective hydrogenation of nitroaromatics under mild reaction conditions. In this work, zinc-modified Ni-Ti catalysts (NixZnyTi1) were fabricated and applied for the hydrogenation of nitroaromatics hydrogenation. It was found that the introduction of zinc effectively increases the surface Ni density, enhances the electronic effect, and improves the interaction between Ni and TiO2, resulting in smaller Ni particle size, more oxygen vacancies, higher dispersion and greater concentration of Ni on the catalyst surface. Furthermore, the electron-rich Niδ– obtained by electron transfer from Zn and Ti to Ni effectively adsorbs and dissociates hydrogen. The results reveal that NixZnyTi1 (Ni0.5Zn0.5Ti1) shows excellent catalytic performance under mild conditions (70 °C and 6 bar). These findings provide a rational strategy for the development of highly active non-noble-metal hydrogenation catalysts.

关键词： bimetal strategy     oxygen vacancy     non-noble metal catalyst     hydrogenation     aromatic nitro compounds    

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Crystal design of bismuth oxyiodide with highly exposed (110) facets on curved carbon nitride for the photocatalytic degradation of pollutants in wastewater

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1125-1138 doi: 10.1007/s11705-021-2116-0

摘要： Crystalline materials with specific facet atomic arrangements and crystal facet structures exhibit unique functions according to their facet effects, quantum size effects and physical and chemical properties. In this study, a novel high-exposure (110) facet of bismuth oxyiodide (BiOI) was prepared (denoted as BiOI-110), and designed as nanosheets rich in oxygen vacancies by crystal facet design and regulation. Graphitic carbon nitride was designed as curved carbon nitride with dibromopyrazine, denoted as DCN, which contributed to a significant structural distortion in plane symmetry and improved the separation of charge carriers. Novel heterostructured BiOI-110/DCN nanosheets with a high-exposure (110) facet and abundant oxygen vacancies were successfully designed to enhance the photocatalytic degradation of organic pollutants. It was demonstrated that complete and tight contact between BiOI-110 and DCN was achieved by changing the size and crystal facet of BiOI. Oxytetracycline (OTC) and methyl blue dyes were used as targets for pollutant degradation, and 85.6% and 96.5% photocatalytic degradation efficiencies, respectively, were observed in the optimal proportion of 7% BiOI-110/DCN. The experimental results and electron spin resonance analysis showed that •O2– and h+ played a major role in the process of pollutant degradation. Additionally, high-resolution liquid chromatography-mass spectrography was used to identify the reaction intermediates of OTC, and the possible degradation pathway of this pollutant was proposed. Finally, the excellent reusability of BiOI-110/DCN nanomaterials was confirmed, providing a new approach for the removal of antibiotics that are difficult to biodegrade. Overall, crystal facet design has been proven to have broad prospects in improving the water environment.

关键词： high-exposure (110) facet     oxygen vacancy-rich     BiOI-110/DCN heterojunction     photocatalytic degradation     visible-light-response    

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Catalytic combustion of methane over a highly active and stable NiO/CeO

Xiuhui Huang, Junfeng Li, Jun Wang, Zeqiu Li, Jiayin Xu

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 534-545 doi: 10.1007/s11705-019-1821-4

摘要： In the last decades, many reports dealing with technology for the catalytic combustion of methane (CH ) have been published. Recently, attention has increasingly focused on the synthesis and catalytic activity of nickel oxides. In this paper, a NiO/CeO catalyst with high catalytic performance in methane combustion was synthesized via a facile impregnation method, and its catalytic activity, stability, and water-resistance during CH combustion were investigated. X-ray diffraction, low-temperature N adsorption, thermogravimetric analysis, Fourier transform infrared spectroscopy, hydrogen temperature programmed reduction, methane temperature programmed surface reaction, Raman spectroscopy, electron paramagnetic resonance, and transmission electron microscope characterization of the catalyst were conducted to determine the origin of its high catalytic activity and stability in detail. The incorporation of NiO was found to enhance the concentration of oxygen vacancies, as well as the activity and amount of surface oxygen. As a result, the mobility of bulk oxygen in CeO was increased. The presence of CeO prevented the aggregation of NiO, enhanced reduction by NiO, and provided more oxygen species for the combustion of CH . The results of a kinetics study indicated that the reaction order was about 1.07 for CH and about 0.10 for O over the NiO/CeO catalyst.

关键词： methane combustion     NiO/CeO2 catalyst     interaction     oxygen vacancy     kinetic study    

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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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FeNi/Al-Ce-O催化剂上的乙烷干重整——组成诱导的金属-载体强相互作用 Article

张涛, 刘志成, 叶迎春, 王毓, 杨贺勤, 高焕新, 杨为民

《工程（英文）》 2022年 第18卷 第11期   页码 173-185 doi: 10.1016/j.eng.2021.11.027

摘要：

在页岩气革命的背景下，乙烷干重整因在化学原料生产和碳减排方面的潜力而备受关注。本研究通过X射线光电子能谱、H2程序升温还原和能量散射X射线谱等手段，揭示了一种组成诱导的金属-载体强相互作用。氧化铈中Al的引入增强了金属与载体之间的相互作用，显著影响了Al-Ce-O载体表面FeNi活性组分的分散度，从而提升了FeNi/Al-Ce-O催化剂的乙烷干重整反应性能。随着载体中Al含量的增加，负载FeNi催化剂的乙烷和二氧化碳的转化率与转换频率（TOF）以及一氧化碳选择性和产率都呈现先增大后减小的趋势，与载体的理论有效表面积（TESA）的变化趋势相同。其中，Al含量为50%的FeNi/Ce-Al0.5催化剂在873 K下具有最好的乙烷干重整反应性能。结合原位傅里叶变换红外光谱（FTIR）分析观察到，Al的引入不仅增加了表面Ce3+和氧空位的含量，同时也促进了表面活性组分的分散，提升了负载FeNi催化剂的乙烷干重整性能。

关键词： 乙烷干重整     金属-载体强相互作用     二氧化碳     氧化铈     氧空位     反应机理    

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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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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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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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标题 作者 时间 类型 操作

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

期刊论文

In situ DRIFTS study of photocatalytic CO 2 reduction under UV irradiation

Jeffrey C. S. WU, Chao-Wei HUANG,

期刊论文

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

期刊论文

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

期刊论文

Catalytic oxidation of CO over Pt/Fe

Zihao Li, Yang Geng, Lei Ma, Xiaoyin Chen, Junhua Li, Huazhen Chang, Johannes W. Schwank

期刊论文

Zinc modification of Ni-Ti as efficient NiZnTi catalysts with both geometric and electronic improvements for hydrogenation of nitroaromatics

期刊论文

Crystal design of bismuth oxyiodide with highly exposed (110) facets on curved carbon nitride for the photocatalytic degradation of pollutants in wastewater

期刊论文

Catalytic combustion of methane over a highly active and stable NiO/CeO

Xiuhui Huang, Junfeng Li, Jun Wang, Zeqiu Li, Jiayin Xu

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

FeNi/Al-Ce-O催化剂上的乙烷干重整——组成诱导的金属-载体强相互作用

张涛, 刘志成, 叶迎春, 王毓, 杨贺勤, 高焕新, 杨为民

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

Multivalent manganese oxides with high electrocatalytic activity for oxygen reduction reaction

Xiangfeng Peng, Zhenhai Wang, Zhao Wang, Yunxiang Pan

期刊论文

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

期刊论文