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N-doped CoAl oxides from hydrotalcites with enhanced Oxygen vacancies for excellent low-temperature propane oxidation

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Journal of Environmental Sciences 2022年第6期34卷 79-89页

作者： Enhui Wu Daifeng Lin Yinye Chen Xiaoshan Feng Kui Niu Yongjin Luo Baoquan Huang Jianbin Qiu Qingrong Qian Qinghua Chen Fujian Key Laboratory of Pollution Control&Resource Reuse Fujian Normal UniversityFuzhou 350007China College of Environmental Science and Engineering Fujian Normal UniversityFuzhou 350007China

A series of nitrogen-doped CoAlO(N-CoAlO)were constructed by a hydrothermal route combined with a controllable NH_(3) treatment strategy.The effects of NH_(3) treatment on the physico-chemical properties and oxidation activities of N-Co AlO catalysts were investigated.In comparison to CoAlO,a smallest content decrease in surface Co^(3+)(serving as active sites)while a largest increased amount of surface Co^(2+)(contributing to oxygen species)are obtained over N-Co AlO/4h among the N-CoAlO catalysts.Meanwhile,a maximum N doping is found over N-CoAlO/4h.As a result,N-CoAlO/4h(under NH_(3) treatment at 400℃ for 4 hr)with rich Oxygen vacancies shows optimal catalytic activity,with a T90(the temperature required to reach a 90% conversion of propane)at 266℃.The more Oxygen vacancies are caused by the co-operative effects of N doping and suitable reduction of Co^(3+) for NCoAlO/4h,leading to an enhanced oxygen mobility,which in turn promotes C_(3)H_(8) total oxidation activity dominated by Langmuir-Hinshelwood mechanism.Moreover,in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTs)analysis shows that N doping facilities the decomposition of intermediate species(propylene and formate)into CO_(2)over the catalyst surface of N-CoAlO/4h more easily.Our reported design in this work will provide a promising way to develop abundant Oxygen vacancies of Co-based catalysts derived from hydrotalcites by a simple NH_(3) treatment.

关键词： Hydrotalcite derived oxides Propane oxidation N doping Co species Oxygen vacancies

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Boosting Oxygen vacancies by modulating the morphology of Au decorated In_(2)O_(3)with enhanced CO_(2)hydrogenation activity to CH_(3)OH

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Journal of Environmental Sciences 2024年第6期140卷 91-102页

作者： Ruxian Hou Jiewen Xiao Qian Wu Tianyu Zhang Qiang Wang Beijing Key Lab for Source Control Technology of Water Pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China Engineering Research Center for Water Pollution Source Control&Eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China

CO_(2)hydrogenation to methanol has become one of the most promising ways for CO_(2)utilization,however,the CO_(2)conversion rate and methanol selectivity of this reaction still need to be improved for industrial application.Here we investigated the structure-activity relationship for CO_(2)conversion to methanol of In_(2)O_(3)-based catalysts by modulating morphology and decorating Au.Three different Au/In_(2)O_(3)catalysts were prepared,their activity follow the sequence of Au/In_(2)O_(3)-nanosphere(Au/In_(2)O_(3)-NS)>Au/In_(2)O_(3)-nanoplate(Au/In_(2)O_(3)-NP)>Au/In_(2)O_(3)-hollow microsphere(Au/In_(2)O_(3)-HM).Au/In_(2)O_(3)-NS exhibited the best performance with good CO_(2)conversion of 12.7%,high methanol selectivity of 59.8%,and large space time yield of 0.32 g CH_(3)OH/(hr·gcat)at 300℃.The high performance of Au/In_(2)O_(3)-NS was considered as the presence of Au.It contributes to the creation of more surface Oxygen vacancies,which further promoted the CO_(2)adsorption and facilitated CO_(2)activation to form the formate intermediates towards methanol.This work clearly suggests that the activity of In_(2)O_(3)catalyst can be effective enhanced by structure engineering and Au decorating.

关键词： CO_(2)hydrogenation Methanol Au/In_(2)O_(3) Morphology Oxygen vacancies

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Ru-based catalysts for efficient CO_(2) methanation:Synergistic catalysis between Oxygen vacancies and basic sites

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Nano Research 2023年第10期16卷 12153-12164页

作者： Chunfen Wang Yonglian Lu Yu Zhang Hui Fu Shuzhuang Sun Feng Li Zhiyao Duan Zhen Liu Chunfei Wu Youhe Wang Hongman Sun Zifeng Yan State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580China School of Chemistry and Chemical Engineering Queen’s University BelfastBelfast BT71NNUK State Key Laboratory of Solidification Processing School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China

The fundamental insights of the reaction mechanism,especially the synergistic effect between Oxygen vacancies and basic sites,are highly promising yet challenging for Ru-based catalysts during carbon dioxide(CO_(2))methanation.Herein,a series of Rubased catalysts were employed to study the mechanism of CO_(2) methanation.It is found that Ru/CeO_(2) catalyst exhibits a much higher CO_(2) conversion(86%)and CH4 selectivity(100%),as well as excellent stability of 30 h due to the existence of abundant Oxygen vacancies and weak basic sites.Additionally,the in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations reveal that the formate formation step dominated the hydrogenation route on Ru/CeO_(2) catalyst,and the b-HCOO^(*)could be the key intermediate due to b-HCOO^(*)is more easily hydrogenated to methane than m-HCOO^(*).The systematic study marks the significance of precise tailoring of the synergistic relationship between Oxygen vacancies and basic sites for achieving the desired performance in CO_(2) methanation.

关键词： Ru-based catalysts Oxygen vacancies basic sites CO_(2)methanation mechanism study

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Pt-surface Oxygen vacancies coupling accelerated photo-charge extraction and activated hydrogen evolution

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Nano Research 2023年第4期16卷 4736-4741页

作者： Fangxu Dai Mingming Zhang Mingzhong Mi Zhenjiang Li Jun Xing Lei Wang Key Laboratory of Eco-chemical Engineering Ministry of EducationCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyShandong Engineering Research Center for Marine Environment Corrosion and Safety ProtectionQingdao 266042China

Semiconductors-based heterogeneous photocatalytic water splitting has been extensively studied,but it still remains challenging to accelerate the separation of electron-hole pairs and facilitate the reaction kinetics.Here we report a general strategy to fabricate highly efficient Pt/TiO_(2)photocatalyst by coupling the Pt co-catalysts and surface Oxygen vacancies(VO)of TiO_(2).TiO_(2)was pre-modified with alkali or alkaline earth metals ion solutions,which produce a large number of surface hydroxyl on TiO_(2).Subsequently,the photodeposited Pt sub-nanoparticles substitute surface hydroxyl and induce surface VO on TiO_(2).The coupling of Pt and surface VO on TiO_(2)can accelerate the extraction of photo-charges through the interaction of Pt-VO-Ti bonds and reduce the hydrogen evolution barrier,thereby promoting the photocatalytic activity.The synthesized Pt-VO-TiO_(2)sample exhibits a photocatalytic hydrogen evolution activity as high as 1.5 L·g^(−1)·h^(−1),which is 2.2 times that of traditional Pt/TiO_(2).Our findings indepth understand the synergistic effect of co-catalysts and defects on photocatalysis and open up new possibilities for achieving robust photocatalytic water splitting.

关键词： Oxygen vacancies co-catalyst surface hydroxyl photocatalytic hydrogen evolution reaction(HER)

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Adjusting Oxygen vacancies in perovskite LaCoO_(3)by electrochemical activation to enhance the hydrogen evolution reaction activity in alkaline condition

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Journal of Energy Chemistry 2023年第1期76卷 226-232,I0006页

作者： Chengrong Wu Yan Sun Xiaojian Wen Jia-Ye Zhang Liang Qiao Jun Cheng Kelvin H.L.Zhang State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina School of Physics University of Electronic Science and Technology of ChinaChengdu 610054SichuanChina

Developing highly-active,earth-abundant non-precious-metal catalysts for hydrogen evolution reaction(HER)in alkaline solution would be beneficial to sustainable energy storage.Perovskite oxides are generally regarded as low-active HER catalysts,due to their inapposite hydrogen adsorption and water dissociation.Here,we report a detailed study on perovskite LaCoO_(3)epitaxial thin films as a model catalyst to significantly enhance the HER performance via an electrochemical activation process.As a result,the overpotential for the activation films to achieve a current density of 0.36 m A/cm^(2)is 238 m V,reduced by more than 200 m V in comparison with that of original samples.Structural characterization revealed the activation process dramatically increases the concentration of Oxygen vacancies(Vo)on the surface of LaCoO_(3).We established the relationship between the electronic structure induced by Vo and the enhanced HER activity.Further theoretical calculations revealed that the Vo optimizes the hydrogen adsorption and dissociation of water on the surface of LaCoO_(3)thin films,thus improving the HER catalytic activity.This work may promote a deepened understanding of perovskite oxides for HER mechanism by Vo adjusting and a new avenue for designing highly active electrochemical catalysts in alkaline solution.

关键词： Hydrogen evolution reaction Perovskite oxides Activation process Oxygen vacancies

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Enhanced performance of Oxygen vacancies on CO_(2) adsorption and activation over different phases of ZrO_(2)

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能源前沿:英文版 2023年第4期17卷 545-554页

作者： Juntian NIU Cunxin ZHANG Haiyu LIU Yan JIN Riguang ZHANG College of Electrical and Power Engineering Taiyuan University of TechnologyTaiyuan030024China State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan030024China

The effect of Oxygen vacancies on the adsorption and activation of CO_(2) on the surface of different phases of ZrO_(2) is investigated by density functional theory(DFT)calculations.The calculations show that the Oxygen vacancies contribute greatly to both the adsorption and activation of CO_(2).The adsorption energy of CO_(2) on the c-ZrO_(2),t-ZrO_(2) and,m-ZrO_(2) surfaces is enhanced to 5,4,and 3 folds with the help of Oxygen vacancies,respectively.Moreover,the energy barrier of CO_(2) dissociation on the defective surfaces of c-ZrO_(2),t-ZrO_(2),and m-ZrO_(2) is reduced to 1/2,1/4,and 1/5 of the perfect surface with the assistance of Oxygen vacancies.Furthermore,the activation of CO_(2) on the ZrO_(2) 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 CO_(2) both kinetically and thermodynamically.These results could provide guidance for the high-efficient utilization of CO_(2) at an atomic scale.

关键词： CO_(2)activation Oxygen vacancies ZrO_(2) different phases

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High-rate performance magnesium batteries achieved by direct growth of honeycomb-like V_(2)O_(5)electrodes with rich Oxygen vacancies

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Nano Research 2023年第4期16卷 4880-4887页

作者： Dongzheng Wu Yichao Zhuang Fei Wang Yang Yang Jing Zeng Jinbao Zhao College of Chemistry and Chemical Engineering State-Province Joint Engineering Laboratory of Power Source Technology for New Energy VehicleState Key Laboratory of Physical Chemistry of Solid SurfacesEngineering Research Center of Electrochemical TechnologyMinistry of EducationCollaborative Innovation Center of Chemistry for Energy MaterialsXiamen UniversityXiamen 361005China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China

Rechargeable magnesium batteries(RMBs)have emerged as a promising next-generation electrochemical energy storage technology due to their superiority of low price and high safety.However,the practical applications of RMBs are severely limited by immature electrode materials.Especially,the high-rate cathode materials are highly desired.Herein,we propose a dualfunctional design of V_(2)O_(5)electrode with rational honeycomb-like structure and rich Oxygen vacancies to enhance the kinetics synergistically.The result demonstrates that Oxygen vacancies can not only boost the intrinsic electronic conductivity of V_(2)O_(5),but also enhance the Mg^(2+)diffusion kinetics inside the cathode,leading to the good high-rate performance.Moreover,ex-situ X-ray diffraction(XRD),transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy(XPS)characterizations reveal that Mg^(2+)is mainly intercalated from the(101)plane of V_(2)O_(5)−X based on the insertion-type electrochemical mechanism;meanwhile,the highly reversible structure evolution during Mg^(2+)insertion/extraction is also verified.This work proposes that the dual-functional design of electrode has a great influence in enhancing the electrochemical performance of cathode materials for RMBs.

关键词： V2O5 rechargeable magnesium batteries Oxygen vacancies kinetics electronic conductivity

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Construction of mesoporous ceria-supported gold catalysts with rich Oxygen vacancies for efficient CO oxidation

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Journal of Rare Earths 2022年第3期40卷 434-442,I0003页

作者： Xin Shen Wang Li Shunmin Ding Xiaohua Ma Shaohua Wu Weiming Xiao Rong Zeng Sanguo Hong Chao Chen Key Laboratory of Jiangxi Province for Environment and Energy Catalysis College of ChemistryNanchang UniversityNanchang 330031China Jiangxi Province Key Laboratory of Polymer Micro/Nano Manufacturing and Devices School of ChemistryBiology and Materials ScienceEast China University of TechnologyNanchang 330013China

Bearing unique redox nature and high oxygen storage capacity,ceria(CeO_(2))has always been a promising CO oxidation catalyst support for gold(Au)catalysts and the like.Herein,a series of Au-CeO_(2)-P(P stands for pH value)samples was prepared by a co-precipitation method with the assistance of an alkaline environment and amino groups functionalized ordered mesoporous polymer(OMP-NH_(2)).Afterward,all samples described above were characterized that the Au-CeO_(2)-P catalysts are made of Au-Ce-O solid solution and Au nanoparticles(NPs)supported on CeO_(2).It turns out that OMP-NH_(2) is not just a simple sacrificial template for mesoporous structure,but also plays an important role as an amino source,explaining the presence of rich Oxygen vacancies.Due to the concentration of Oxygen vacancies in Au-Ce-O solid solution is the key factor for the oxygen mobility of CO oxidation,the catalytic results also demonstrate that the catalytic activity of Au-CeO_(2)-P catalysts is related to the concentration of their Oxygen vacancies.Moreover,Au-CeO_(2)-9.6 with a highest concentration of Oxygen vacancies(as high as 13.98%)in Au-CeO_(2)-P catalysts exhibits the best catalytic activity(complete conversion at 10℃).

关键词： Ceria Oxygen vacancies Au-Ce-O solid Solution Amino groups functionalized ordered mesoporous polymer CO oxidation Rare earths

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CeO_(2) nanoparticles with Oxygen vacancies decorated N-doped carbon nanorods:A highly efficient catalyst for nitrate electroreduction to ammonia

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Nano Research 2022年第10期15卷 8914-8921页

作者： Zerong Li Zhiqin Deng Ling Ouyang Xiaoya Fan Longcheng Zhang Shengjun Sun Qian Liu Abdulmohsen Ali Alshehri Yonglan Luo Qingquan Kong Xuping Sun Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province School of Chemistry and Chemical engineeringChina West Normal UniversityNanchong 637002China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China Institute for Advanced Study Chengdu UniversityChengdu 610106China Chemistry Department Faculty of ScienceKing Abdulaziz UniversityP.O.Box 80203Jeddah 21589Saudi Arabia College of Chemistry Chemical Engineering and Materials ScienceShandong Normal UniversityJinan 250014China

Electrocatalytic nitrate reduction reaction(NO_(3)−RR)emerges as a highly efficient approach toward ammonia synthesis and degrading NO_(3)−contaminant.In our study,CeO_(2) nanoparticles with Oxygen vacancies(VO)decorated N-doped carbon nanorods on graphite paper(CeO_(2)−x@NC/GP)were demonstrated as a highly efficient NO_(3)−RR electrocatalyst.The CeO_(2)−x@NC/GP catalyst manifests a significant NH_(3 )yield up to 712.75μmol·h^(−1)·cm^(−2) at−0.8 V vs.reversible hydrogen electrode(RHE)and remarkable Faradaic efficiency of 92.93%at−0.5 V vs.RHE under alkaline conditions,with excellent durability.Additionally,an assembled Zn-NO_(3)−battery with CeO_(2)−x@NC/GP as cathode accomplishes a high-power density of 3.44 mW·cm^(−2) and a large NH3 yield of 145.08μmol·h^(−1)·cm^(−2).Density functional theory results further expose the NO_(3)−reduction mechanism on CeO_(2)(111)surface with VO.

关键词： CeO_(2)−x nanoparticles Oxygen vacancies electrochemical NO_(3)−reduction ammonia synthesis electrocatalysis

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Au atoms doped in Ti_(3)C_(2)T_(x)MXene:Benefiting recovery of Oxygen vacancies towards photocatalytic aerobic oxidation

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Nano Research 2022年第4期15卷 2862-2869页

作者： Kaifu Yu Sanmei Wang Qi Li Tingting Hou Yue Xin Rong He Wenhua Zhang Shuquan Liang Liangbing Wang Wenkun Zhu State Key Laboratory of Environment-friendly Energy Materials National Co-innovation Center for Nuclear Waste Disposal and Environmental SafetySchool of National Defence Science&TechnologySouthwest University of Science and TechnologyMianyang 621010China State Key Laboratory for Powder Metallurgy Key Laboratory of Electronic Packing and Advanced Functional Materials of Hunan ProvinceSchool of Materials Science and EngineeringCentral South UniversityChangsha 410083China Hefei National Laboratory for Physical Sciences at the Microscale Synergetic Innovation Centre of Quantum Information&Quantum PhysicsCAS Key Laboratory of Materials for Energy ConversionUniversity of Science and Technology of ChinaHefei 230026China

Photocatalytic aerobic oxidation by using oxygen molecules(O_(2))as green and low-cost oxidants is of great attraction,where the introduction of irradiation has been proved as an efficient strategy to lower reaction temperature as well as promote catalytic performance.Moreover,the Oxygen vacancies(OVs)of catalyst are highly active sites to adsorb and activate O_(2)during photocatalytic aerobic oxidation.However,OVs are easily blocked by oxygen atoms from active oxygen species during the catalytic process,leading to the deactivation of catalysis.Herein,a promising catalyst toward photocatalytic aerobic oxidation was successfully developed by recovering the OVs through doping Au atoms into Ti_(3)C_(2)T_(x)MXene(Au/Ti_(3)C_(2)T_(x)).Impressively,Au/Ti_(3)C_(2)T_(x)exhibited remarkable activity under full-spectrum irradiation towards photooxidation of methyl phenyl sulfide(MPS)and methylene blue(MB),attaining a conversion of>90%at room temperature.Moreover,Au/Ti_(3)C_(2)T_(x)also manifested remarkable stability by maintaining>95%initial activity after 10 successive reaction rounds.Further mechanistic studies indicated that the OVs of Au/Ti_(3)C_(2)T_(x)served as the active centers to efficiently adsorb and activate O_(2).More importantly,the doped Au atoms of Au/Ti_(3)C_(2)T_(x)were conducive to the recovery of OVs during photocatalytic process from the results of theoretical and experimental aspects.The recovered OVs of Au/Ti_(3)C_(2)T_(x)continuously and efficiently activated O_(2),directly contributing to the remarkable catalytic activity and stability.

关键词： Oxygen vacancies doped Au atoms Ti_(3)C_(2)T_(x)MXene photocatalysis aerobic oxidation

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