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Advancements on metal oxide semiconductor photocatalysts in photo-electrochemical conversion of carbon dioxide into fuels and other useful products

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Frontiers in Energy 2024年第2期18卷 187-205页

作者： Jai PRAKASH zhangsen chen Shakshi SAINI Gaixia ZHANG Shuhui SUN Department of Chemistry National Institute of Technology HamirpurHamirpur 177005India Institut National de la Recherche Scientifique(INRS) Centre Énergie Matériaux TélécommunicationsVarennes J3X 1P7Canada Department of Chemistry Indian Institute of Technology MandiHimachal PradeshIndia Department of Electrical Engineering École de Technologie SupérieureMontréal H3C 1K3Canada

Due to its fascinating and tunable optoelectronic properties,semiconductor nanomaterials are the best choices for multidisciplinary applications.Particularly,the use of semiconductor photocatalysts is one of the promising ways to harness solar energy for useful applications in the field of energy and environment.In recent years,metal oxide-based tailored semiconductor photocatalysts have extensively been used for photocatalytic conversion of carbon dioxide(CO_(2))into fuels and other useful products utilizing solar energy.This is very significant not only from renewable energy consumption but also from reducing global warming point of view.Such current research activities are promising for a better future of society.The present mini-review is focused on recent developments(2–3 years)in metal oxide semiconductor hybrid photocatalysts-based photo-electrochemical conversion of CO_(2)into fuels and other useful products.First,general mechanism of photo-electrochemical conversion of CO_(2)into fuels or other useful products has been discussed.Then,various metal oxide-based emerging hybrid photocatalysts including tailoring of their morphological,compositional,and optoelectronic properties have been discussed with emphasis on their role in enhancing photoelectrochemical efficienty.Afterwards,mechanism of their photo-electrochemical reactions and applications in CO_(2)conversion into fuels/other useful products have been discussed.Finally,challenges and future prospects have been discussed followed by a summary.

关键词： metal-oxide semiconductors nanohybrid photocatalysts photo-electrochemical CO_(2)conversion tailoring morphology fuels challenges and future prospects

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Atomically Dispersed Fe-Co Bimetallic Catalysts for the Promoted Electroreduction of Carbon Dioxide

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Nano-Micro Letters 2022年第2期14卷 79-93页

作者： zhangsen chen Gaixia Zhang Yuren Wen Ning chen Weifeng chen Tom Regier James Dynes Yi Zheng Shuhui Sun Institut National de la Recherche Scientifique-Énergie Matériaux et Télécommunications VarennesQC J3X 1P7Canada School of Materials Science and Engineering University of Science and Technology100083 BeijingPeople’s Republic of China Canadian Light Source University of SaskatchewanSaskatoonSK S7N 2V3Canada Research Institute of Photocatalysis State Key Laboratory of Photocatalysis on Energy and EnvironmentFuzhou UniversityFuzhou 350116People’s Republic of China

The electroreduction reaction of CO_(2)(ECO_(2)RR)requires high-performance catalysts to convert CO_(2)into useful chemicals.Transition metal-based atomically dispersed catalysts are promising for the high selectivity and activity in ECO_(2)RR.This work presents a series of atomically dispersed Co,Fe bimetallic catalysts by carbonizing the Fe-introduced Co-zeolitic-imidazolate-framework(C-Fe-Co-ZIF)for the syngas generation from ECO_(2)RR.The synergistic effect of the bimetallic catalyst promotes CO production.Compared to the pure C-Co-ZiF,C-Fe-Co-ZIF facilitates CO production with a CO Faradaic efficiency(FE)boost of 10%,with optimal FE_(CO)of 51.9%,FE_(H_(2))of 42.4%at-0.55 V,and CO current density of 8.0 mA cm^(-2)at-0.7 V versus reversible hydrogen electrode(RHE).The H_(2)/CO ratio is tunable from 0.8 to 4.2 in a wide potential window of-0.35 to-0.8 V versus RHE.The total FE_(CO+H_(2))maintains as high as 93%over 10 h.The proper adding amount of Fe could increase the number of active sites and create mild distortions for the nanoscopic environments of Co and Fe,which is essential for the enhancement of the CO production in ECO_(2)RR.The positive impacts of Cu-Co and Ni-Co bimetallic catalysts demonstrate the versatility and potential application of the bimetallic strategy for ECO_(2)RR.

关键词： CO_(2)reduction Electrocatalysis Syngas production Cobalt Iron Bimetallic catalysts

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Atomically Dispersed Transition Metal-Nitrogen-Carbon Bifunctional Oxygen Electrocatalysts for Zinc-Air Batteries:Recent Advances and Future Perspectives

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Nano-Micro Letters 2022年第2期14卷 257-281页

作者： Fang Dong Mingjie Wu zhangsen chen Xianhu Liu Gaixia Zhang Jinli Qiao Shuhui Sun Institut National de La Recherche Scientifique(INRS)-CentreÉnergie Matériaux Télécommunications VarennesQC J3X 1P7Canada Key Laboratory of Materials Processing and Mold Ministry of EducationZhengzhou UniversityZhengzhou 450002People’s Republic of China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringShanghai Innovation Institute for MaterialsDonghua UniversityShanghai 201620People’s Republic of China Engineering Research Center of Nano Geomaterials of Ministry of EducationChina University of GeosciencesWuhan 430074People’s Republic of China

Rechargeable zinc-air batteries(ZABs)are currently receiving extensive attention because of their extremely high theoretical specific energy density,low manufacturing costs,and environmental friendliness.Exploring bifunctional catalysts with high activity and stability to overcome sluggish kinetics of oxygen reduction reaction and oxygen evolution reaction is critical for the development of rechargeable ZABs.Atomically dispersed metal-nitrogen-carbon(M-N-C)catalysts possessing prominent advantages of high metal atom utilization and electrocatalytic activity are promising candidates to promote oxygen electrocatalysis.In this work,general principles for designing atomically dispersed M-N-C are reviewed.Then,strategies aiming at enhancing the bifunctional catalytic activity and stability are presented.Finally,the challenges and perspectives of M-N-C bifunctional oxygen catalysts for ZABs are outlined.It is expected that this review will provide insights into the targeted optimization of atomically dispersed M-N-C catalysts in rechargeable ZABs.

关键词： Atomically dispersed metal-nitrogen-carbon Oxygen evolution reaction(OER) Oxygen reduction reaction(ORR) Bifunctional oxygen electrocatalysts Zinc-air batteries(ZABs)

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Interface Engineering of NixSy@MnOxHy Nanorods to Efficiently Enhance Overall-Water-Splitting Activity and Stability

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Nano-Micro Letters 2022年第7期14卷 246-262页

作者： Pan Wang Yuanzhi Luo Gaixia Zhang zhangsen chen Hariprasad Ranganathan Shuhui Sun Zhicong Shi Institute of Batteries School of Materials and EnergyGuangdong University of TechnologyGuangzhou 510006People’s Republic of China Énergie Matériaux Télécommunications Research Centre Institut National de La Recherche Scientifique(INRS)VarennesQuébec J3X 1P7Canada The Key Laboratory of Fuel Cell Technology of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510641People’s Republic of China

Exploring highly active and stable transition metal-based bifunctional electrocatalysts has recently attracted extensive research interests for achieving high inherent activity, abundant exposed active sites, rapid mass transfer, and strong structure stability for overall water splitting. Herein, an interface engineering coupled with shell-protection strategy was applied to construct three-dimensional(3D) core-shell NixSy@MnOxHy heterostructure nanorods grown on nickel foam(NixSy@MnOxHy/NF) as a bifunctional electrocatalyst. NixSy@MnOxHy/NF was synthesized via a facile hydrothermal reaction followed by an electrodeposition process. The X-ray absorption fine structure spectra reveal that abundant Mn-S bonds connect the heterostructure interfaces of N ixSy@MnOxHy, leading to a strong electronic interaction, which improves the intrinsic activities of hydrogen evolution reaction and oxygen evolution reaction(OER). Besides, as an efficient protective shell, the MnOxHy dramatically inhibits the electrochemical corrosion of the electrocatalyst at high current densities, which remarkably enhances the stability at high potentials. Furthermore, the 3D nanorod structure not only exposes enriched active sites, but also accelerates the electrolyte diffusion and bubble desorption. Therefore, NixSy@MnOxHy/NF exhibits exceptional bifunctional activity and stability for overall water splitting, with low overpotentials of 326 and 356 mV for OER at 100 and 500 mA cm^(–2), respectively, along with high stability of 150 h at 100 mA cm^(–2). Furthermore, for overall water splitting, it presents a low cell voltage of 1.529 V at 10 mA cm^(–2), accompanied by excellent stability at 100 mA cm^(–2) for 100 h. This work sheds a light on exploring highly active and stable bifunctional electrocatalysts by the interface engineering coupled with shell-protection strategy.

关键词： Interface engineering Protective shell Manganese compound Nickel sulfides Bifunctional Water splitting

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Advanced semiconductor catalyst designs for the photocatalytic reduction of CO_(2)

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Materials Reports(Energy) 2023年第2期3卷 27-42,I0002页

作者： zhangsen chen Gaixia Zhang Siyi Cao Guozhu chen Cuncheng Li Ricardo IzquierdoShuhui Sun Institut National de la Recherche Scientifique–Centre Energie Materiaux Telecommunications VarennesQuebecJ3X 1P7Canada Department of Electrical Engineering Ecolede Technologie Superieure(ETS)MontrealQuebecH3C 1K3Canada School of Chemistry and Chemical Engineering University of JinanJinan250022PR China

Using clean solar energy to reduce CO_(2)into value-added products not only consumes the over-emitted CO_(2)that causes environmental problems,but also generates fuel chemicals to alleviate energy crises.The photocatalytic CO_(2)reduction reaction(PCO_(2)RR)relies on the semiconductor photocatalysts that suffer from high recombination rate of the photo-generated carriers,low light harvesting capability,and low stability.This review explores the recent discoveries on the novel semiconductors for PCO_(2)RR,focusing on the rational catalyst design strategies(such as surface engineering,band engineering,hierarchical structure construction,single-atom catalysts,and biohybrid catalysts)that promote the catalytic performance of semiconductor catalysts on PCO_(2)RR.The advanced characterization techniques that contribute to understanding the intrinsic properties of the photocatalysts are also discussed.Lastly,the perspectives on future challenges and possible solutions for PCO_(2)RR are presented.

关键词： Photoreduction of CO_(2) Semiconductor catalysts Photocatalyst modification Heterojunction construction Catalytic efficiency Activity Environmental and sustainable applications

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PtCoNi ternary intermetallic compounds anchored on Co,Ni and N co-doped mesoporous carbon:Synergetic effect between PtCoNi nanoparticles and doped mesoporous carbon promotes the catalytic activity

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Journal of Energy Chemistry 2023年第3期78卷 340-349,I0010页

作者： Chaozhong Li Weiyue Zhao Xueyi Lu zhangsen chen Bing Han Xiaorong Zhang Jiaxiang chen Yijia Shao Junlang Huo Yuexiang Zhu Yonghong Deng Shuhui Sun Shijun Liao The Key Laboratory of Fuel Cell Technology of Guangdong Province&The Key Laboratory of New Energy Technology of Guangdong Universities School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510641GuangdongChina School of Materials Sun Yat-sen UniversityShenzhen 518107GuangdongChina Centre énergie Matériaux et TélécommunicationsInstitute National de la Recherche ScientifiqueVarennesQuébec J3X 1P7Canada Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055GuangdongChina

Highly active and robust electrocatalysts are desired for proton exchange membrane fuel cells.Pt-based intermetallic compounds(IMCs) have been recognized as one of the most promising low-platinum catalysts for fuel cells(FCs).Herein,we report a high-performance IMCs by anchoring ordered PtCoNi ternary nanoparticles on the N,Co and Ni co-doped dodecahedral mesoporous carbon(DMC).While the introduced Co and Ni participate in the formation of PtCoNi IMCs,some of them are doped in the mesoporous carbon and coordinated by N to form Co-N_(y)/Ni-N_(z)dual active centers,which further enhances the electrocatalytic activity towards oxygen reduction reaction.Moreover,the addition of Ni results in a negative shift of the d-band center of Pt as compared to the Pt/DMC and Pt_(3)Co/DMC,making it easier to adsorb oxygen on the surface.As expected,our optimal sample Pt_(3)Co_(0.7)Ni_(0.3)/DMC exhibits excellent performance with mass activity and specific activity of 1.32 A mgPt-1and 1.98 mA cm^(-2)at 0.9 V,which are 7.33and 6.19 times that of commercial Pt/C,respectively.The Pt_(3)Co_(0.7)Ni_(0.3)/DMC also reveals much better cathodic performance in an H2-air single fuel cell than commercial Pt/C catalyst with a power density of0.802 W cm^(-2).This work provides critical sights into constructing efficient catalysts by ternary intermetallic strategy and synergetic effect between active components and support.

关键词： Ternary intermetallic compounds Oxygen reduction reaction Fuel cell Catalyst

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Atomically Dispersed Ruthenium Catalysts with Open Hollow Structure for Lithium-Oxygen Batteries

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Nano-Micro Letters 2024年第2期16卷 154-164页

作者： Xin chen Yu Zhang Chang chen Huinan Li Yuran Lin Ke Yu Caiyun Nan chen chen Beijing Advanced Innovation Center for Materials Genome Engineering Institute of Solid State ChemistryUniversity of Science and Technology BeijingBeijing 100083People’s Republic of China Engineering Research Center of Advanced Rare Earth Materials Department of ChemistryTsinghua UniversityBeijing 100084People’s Republic of China Beijing Key Laboratory of Energy Conversion and Storage Materials Institution College of ChemistryBeijing Normal UniversityBeijing 100875People’s Republic of China

Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult decomposition of discharge products at present.Here,we have developed N-doped carbon anchored atomically dispersed Ru sites cathode catalyst with open hollow structure(h-RuNC)for Lithium–oxygen battery.On one hand,the abundance of atomically dispersed Ru sites can effectively catalyze the formation and decomposition of discharge products,thereby greatly enhancing the redox kinetics.On the other hand,the open hollow structure not only enhances the mass activity of atomically dispersed Ru sites but also improves the diffusion efficiency of catalytic molecules.Therefore,the excellent activity from atomically dispersed Ru sites and the enhanced diffusion from open hollow structure respectively improve the redox kinetics and cycling stability,ultimately achieving a high-performance lithium–oxygen battery.

关键词： Atomically dispersed Open hollow structure Discharge product Lithium Oxygen battery

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Advances in the application of hydrogel-based scaffolds for tendon repair

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Genes & Diseases 2024年第4期11卷 296-313页

作者： Renqiang chen Fanglin chen Kenian chen Jian Xu Department of Orthopedics The First Affiliated HospitalZhejiang University School of MedicineHangzhouZhejiang 310003China Department of Orthopedics The Fourth Affiliated Hospital of Guangxi Medical UniversityLiuzhou Guangxi 545005China

Tendon injuries often lead to joint dysfunction due to the limited self-regeneration capacity of tendons.Repairing tendons is a major challenge for surgeons and imposes a signif-icant financial burden on society.Therefore,there is an urgent need to develop effective stra-tegies for repairing injured tendons.Tendon tissue engineering using hydrogels has emerged as a promising approach that has attracted considerable interest.Hydrogels possess excellent biocompatibility and biodegradability,enabling them to create an extracellular matrix-like growth environment for cells.They can also serve as a carrier for cells or other substances to accelerate tendon repair.In the past decade,numerous studies have made significant prog-ress in the preparation of hydrogel scaffolds for tendon healing.This review aims to provide an overview of recent research on the materials of hydrogel-based scaffolds used for tendon tis-sue engineering and discusses the delivery systems based on them.

关键词： Application Hydrogel-based Repairscaffolds Review Tendon injury Tissue engineering

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Photodegradation of xylene isomers:Kinetics,mechanism,secondary pollutant formation potential and health risk evaluation

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Journal of Environmental Sciences 2024年第2期136卷 658-669页

作者： Xiaoyan chen Weikun Zhu Sufen Feng Jiangyao chen Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control Guangdong Technology Research Center for Photocatalytic Technology Integration and Equipment EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangzhou Key Laboratory of Environmental Catalysis and Pollution Control Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and HealthSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

Photodegradation technology has been widely applied in the purification of industrial aromatic hydrocarbons.However,whether this technology efficiently removes the pollutants to prevent secondary pollution and health risk is still unclear.Here,the photodegradation processes of three xylenes were compared under designed reaction atmospheres and light sources.Xe lamp showed poor photodegradation ability toward xylenes,no matter in N_(2) or N_(2)+O_(2)system,while much higher photodegradation performance of xylenes were obtained under ultraviolet(UV)and vacuum ultraviolet(VUV)irradiation,especially in N_(2)+O_(2)+VUV system,where 97.9%of m-xylene,99.0%of o-xylene or 87.5%of p-xylene with the initial concentration of 860 mg/m^(3) was removed within 240 min.The xylenes underwent three processes of photo-isomerization,photodecomposition and photo-oxidation to produce intermediates of aromatics,alkanes and carbonyls.Among them,the photo-isomerization products showed the highest concentration percentage(e.g.,≥50%in o-xylene system),confirming that photo-isomerization reaction was the dominated photodegradation process of xylenes.Moreover,these isomerized products not only contributed about 97%and91%to the formation potential of O3(OFP)and secondary organic aerosols(SOAFP),but also displayed obvious non-carcinogenic risk,although one of photodecomposition product—benzene showed the highest occupational exposure risk.Therefore,the secondary pollution and health risks of photodegradation products of xylenes were non-ignorable,although the OFP,SOAFP and health risks of the generated products reduced at least 4.5 times in comparison with that of the degraded xylenes.The findings are helpful for the appropriate application of this technology in the purification of industrial organic waste gas.

关键词： Isomer aromatics Photodegradation Ozone formation Secondary organic aerosols Health risk

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Isotopic characteristics and source analysis of atmospheric ammonia during agricultural periods in the Xichuan area of the Danjiangkou Reservoir

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Journal of Environmental Sciences 2024年第2期136卷 460-469页

作者： Xiaoshu chen Tongqian Zhao Chunyan Xiao Xiaoming Guo Feihong chen Institute of Resources and Environment Henan Polytechnic UniversityJiaozuo 454000China

Nitrogen deposition is an important means of exogenous nitrogen input in reservoir water.Agricultural activities around the reservoir lead to a sharp increase in the concentration of ammonia in the atmosphere,which poses a threat to the reservoir water body.Clarifying the contribution of agricultural ammonia release to atmospheric NH_(x)(gaseous NH_(3)and particulate NH_(4)^(+)),in the reservoir area can provide a theoretical foundation for local reactive nitrogen control.We collected atmospheric NH_(3)and NH_(4)^(+)samples during the agricultural periods and analyzed the isotopic characteristics of atmospheric NH_(x)and the contribution rates of different ammonia sources in the Xichuan area of the Danjiangkou Reservoir.The results showed that the initialδ~(15)N values of NH_(3)(-30.0‰to–7.2‰)and particulate NH_(4)^(+)(–33‰to+4.9‰for finer and coarser particles,respectively)are different,and their contribution ratios from dissimilar ammonia sources are also different,among which NH_(4)^(+)is more susceptible to meteorological factors.However,since the atmospheric NH_(x)in the Xichuan area is mainly gaseous NH_(3),the final sources of atmospheric ammonia nitrogen source depend on gaseous NH_(3).Agricultural sources(59%-74%)were the main NH_(3)sources in this area.Among them,the fertilizer use emission was dominant;it had the highest contribution rate in summer during the agricultural period and a more prominent impact in areas with less human interference.Reasonable regulation of the application of high-ammonia releasing fertilizer,especially during the agricultural period in summer,is an effective way to reduce the threat of atmospheric ammonia to water health.

关键词： Danjiangkou reservoir Atmospheric ammonia nitrogen Isotope Ammonia source analysis Agricultural sources

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