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Co/CoO heterojunction rich in oxygen vacancies introduced by O2 plasma embedded in mesoporous walls of carbon nanoboxes covered with carbon nanotubes for rechargeable zinc-air battery

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Carbon Energy 2024年第7期6卷 14-25页

作者： Leijun Ye Weiheng Chen Zhong-Jie Jiang Zhongqing Jiang key laboratory of Optical Field Manipulation of Zhejiang Province Department of PhysicsZhejiang Sci-Tech UniversityHangzhouChina department of Mechanical Engineering Ningbo University of TechnologyNingboChina Guangzhou key laboratory for surface chemistry of Energy Materials Guangdong Engineering and Technology Research Center for Surface Chemistry of Energy MaterialsCollege of Environment and EnergySouth China University of TechnologyGuangzhouChina

Herein,Co/CoO heterojunction nanoparticles(NPs)rich in oxygen vacancies embedded in mesoporous walls of nitrogen-doped hollow carbon nanoboxes coupled with nitrogen-doped carbon nanotubes(P-Co/CoOV@NHCNB@NCNT)are well designed through zeolite-imidazole framework(ZIF-67)carbonization,chemical vapor deposition,and O_(2) plasma *** a result,the threedimensional NHCNBs coupled with NCNTs and unique heterojunction with rich oxygen vacancies reduce the charge transport resistance and accelerate the catalytic reaction rate of the P-Co/CoOV@NHCNB@NCNT,and they display exceedingly good electrocatalytic performance for oxygen reduction reaction(ORR,halfwave potential[EORR,1/2=0.855 V *** hydrogen electrode])and oxygen evolution reaction(OER,overpotential(η_(OER,10)=377mV@10mA cm^(−2)),which exceeds that of the commercial Pt/C+RuO_(2) and most of the formerly reported ***,both the aqueous and flexible foldable all-solid-state rechargeable zinc-air batteries(ZABs)assembled with the P-Co/CoOV@NHCNB@NCNT catalyst reveal a large maximum power density and outstanding long-term cycling ***-principles density functional theory calculations show that the formation of heterojunctions and oxygen vacancies enhances conductivity,reduces reaction energy barriers,and accelerates reaction kinetics *** work opens up a new avenue for the facile construction of highly active,structurally stable,and cost-effective bifunctional catalysts for ZABs.

关键词： heterojunction oxygen evolution/reduction reaction oxygen vacancies rechargeable zinc–air battery three‐dimensional nitrogen‐doped hollow carbon nanoboxes

Boosting High-Voltage Practical Lithium Metal Batteries with Tailored Additives

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Nano-Micro Letters 2024年第12期16卷 23-41页

作者： Jinhai You Qiong Wang Runhong Wei Li Deng Yiyang Hu Li Niu Jingkai Wang Xiaomei Zheng Junwei Li Yao Zhou Jun-Tao Li College of Energy Xiamen UniversityXiamen 361005People’s Republic of China Magnetism key laboratory of Zhejiang Province College of Materials and ChemistryChina Jiliang UniversityHangzhou 310018People’s Republic of China laboratory for Soft Matter and Biophysics Department of Physics and AstronomyKU Leuven3001 LeuvenBelgium state key Lab of physical chemistry of solid surface College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005People’s Republic of China department of Chemical Engineering KU LeuvenCelestijnenlaan 200F3001 LeuvenBelgium College of chemistry and Chemical Engineering Northwest Normal UniversityLanzhou 730070GansuPeople’s Republic of China

The lithium(Li)metal anode is widely regarded as an ideal anode material for high-energy-density ***,uncontrolled Li dendrite growth often leads to unfavorable interfaces and low Coulombic efficiency(CE),limiting its broader ***,an ether-based electrolyte(termed FGN-182)is formulated,exhibiting ultra-stable Li metal anodes through the incorporation of LiFSI and LiNO3 as dual *** synergistic effect of the dual salts facilitates the formation of a highly robust SEI film with fast Li+transport ***,Li||Cu half cells exhibit an average CE reaching up to 99.56%.In particular,pouch cells equipped with high-loading lithium cobalt oxide(LCO,3 mAh cm^(-2))cathodes,ultrathin Li chips(25μm),and lean electrolytes(5 g Ah-1)demonstrate outstanding cycling performance,retaining 80%capacity after 125 *** address the gas issue in the cathode under high voltage,cathode additives 1,3,6-tricyanohexane is incorporated with FGN-182;the resulting high-voltage LCO||Li(4.4 V)pouch cells can cycle steadily over 93 *** study demonstrates that,even with the use of ether-based electrolytes,it is possible to simultaneously achieve significant improvements in both high Li utilization and electrolyte tolerance to high voltage by exploring appropriate functional additives for both the cathode and anode.

关键词： Li metal anode Li dendrites LiNO_(3) 1,3,6-tricyanohexane Pouch cells

How interfacial electron-donating defects influence the structure and charge of gold nanoparticles on TiO_(2)support

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Nano Research 2024年第7期17卷 5965-5974页

作者： Guang-Jie Xia Yu Fu Wei Cao Jun Li Yang-Gang Wang department of chemistry and Guangdong Provincial key laboratory of Catalysis Southern University of Science and TechnologyShenzhen 518055China School of physical Sciences Great Bay UniversityDongguan 523000China department of chemistry Tsinghua UniversityBeijing 100084China

The reduction degree of TiO_(2)support is critical to the performances of metal *** many previous theoretical calculations,only the bridge oxygen vacancy(Ov)was considered as the electron-donating defect on reduced rutile TiO_(2)(r-TiO_(2−x))***,titanium adatoms(Tiad.),oxidized titanium islands(***),and acid hydroxyls(ObrH)also exist at the metal/support *** conducting density functional theory(DFT)calculations and ab initio molecular dynamics(AIMD)simulations,we compared r-TiO_(2−x)surfaces with Ov,Tiad.,***,and ObrH sites loaded with Au nanoparticles(NPs).The results showed the Au NPs were oxygen-phobic but titanium-philic,resulting in wetting of Ov and *** short contact with *** and *** Bader charges of Au NPs(QM)showed a good linear relationship with the ideal number of donating electrons(Ne)from the defective sites(QM=−KeNe+QM,S),demonstrating the intrinsic electron allocation at the *** Ov,Tiad.,and *** exhibited similar slopes(Ke),relatively steeper than that of *** means in the scope of Au NP charge state,the *** *** have a close electron-donating ability with Ov,but the ObrH donates relatively fewer *** linear relationship can be extended approximately to other *** higher the metal work function,the steeper the Ke for easier electron donation from defective *** stronger the metal oxygen affinity,the more positive the intercept(QM,S).That explains the easy generation of metallic or negative Pt and Au NPs on r-TiO_(2−x),but hard for Cu and Zn in *** provides theoretical guidance for regulating the charge of metal NPs over TiO_(2−x)supports.

关键词： metal-support interaction titanium oxide oxygen vacancy surface hydroxyl titanium adatom

Microfluidic-based isolation of circulating tumor cells with high-efficiency and high-purity

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Chinese Chemical Letters 2024年第8期35卷 101-111页

作者： Feng Wu Xuemin Kong Yixuan Liu Shuli Wang Zhong Chen Xu Hou Fujian Engineering Research Center for solid-state Lighting Department of Electronic ScienceSchool of Electronic Science and EngineeringXiamen UniversityXiamen 361005China College of Physics and New Energy Xuzhou University of TechnologyXuzhou 221018China state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China College of physical Science and Technology Xiamen UniversityXiamen 361005China Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China

The isolation of circulating tumor cells(CTCs)from complex biological samples is of paramount signifi-cance for advancing cancer diagnosis,prognosis,and ***,the low concentration of CTCs and nonspecific adhesion of white blood cells(WBCs)present challenges that hinder the efficiency and purity of captured ***-based strategies utilize precise fluid control at the micron level to incorporate specific micro/nanostructures or recognition molecules,enabling effective CTCs ***,by employing surface modification designs that exhibit exceptional anti-adhesion properties against WBCs,the purity of isolated CTCs can be further *** review offers an in-depth explo-ration of recent advancements,challenges,and opportunities associated with microfluidic-based CTCs iso-lation from biological ***,we will comprehensively introduce the microfluidic-based strate-gies for achieving high-efficiency CTCs isolation,which includes the morphological design of microchan-nels for physical force-based CTCs isolation and the specific modification of microchannel surfaces for affinity-based CTCs ***,a review of recent research advances in microfluidic-based high-purity CTCs isolation is presented,focusing on strategies that decrease the nonspecific adhesion of WBCs through surface micro-/nanostructure construction or chemical and biological ***,we will summarize the article by providing the prospective opportunities and challenges for the future development of microfluidic-based CTCs isolation.

关键词： Microfluidics Isolation Circulating tumor cells High-efficiency High-purity

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Enhanced electrochemical performance of nanoscale single crystal NMC811 modification by coating LiNbO_(3)

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Chinese Chemical Letters 2024年第5期35卷 514-518页

作者： Fengyu Zhang Yali Liang Zhangran Ye Lei Deng Yunna Guo Ping Qiu Peng Jia Qiaobao Zhang Liqiang Zhang Clean Nano Energy Center state key laboratory of Metastable Materials Science and Technology Yanshan UniversityQinhuangdao 066004China School of New Energy and Materials China University of Petroleum BeijingBeijing 102249China Hebei key laboratory of Applied chemistry College of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004China state key laboratory of physical chemistry of solid surfaces College of MaterialsXiamen UniversityXiamen 361005China

Single crystallization is an important strategy to resolve intergranular cracks and unnecessary side reactions with electrolytes in layered transition metal oxide cathodes LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811).Due to the limitations of high-temperature sintering and multi-step calcination,single crystal NMC811 generally shows irregular particles with a size of 2-3μ***,the prolonged Li-ion diffusion pathway and the stress generated by the uneven de-/intercalation sluggish Li-ion diffusion kinetics,what is more,cause structural damage such as intragranular cracks.A slow Li extraction rate or particle size reduction will ameliorate the structural damage and improve the cycling *** the most promising cathodes for next-generation power batteries,NMC811 required fast charge performance and cycle *** size reduction appears to be the displacement *** is an effective strategy to mitigate intragranular cracks of single crystal ***,the serious aggregation and increased specific surface area become new *** this article,we synthesized monodisperse nanoscale single crystal NMC811 by molten salt method and modified the surface by LiNbO3 *** electrochemical performance shows that nanoscale single crystal NMC811 has faster kinetic and higher capacity retention,so the strategy of combining nanonization and surface coating is an alternative way to prepare high specific capacity and cycle stable single crystal NMC811.

关键词： Ni-rich NMC811 Molten salt method Nanonization surface coating Micron cracks

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Core-shell nanoparticle enhanced Raman spectroscopy in situ probing the composition and evolution of interfacial species on PtCo surfaces

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Nano Research 2024年第6期17卷 4687-4692页

作者： Jing Liu Han-Liang Zhong Xiangyu Li Mu-Fei Yue Wei-Min Yang Xueqiu You Jing-Hua Tian Yao-Hui Wang Jian-Feng Li Fujian Provincial key laboratory of Oceanic Information Perception and Intelligent Processing School of Ocean Information EngineeringJimei UniversityXiamen 361021China College of chemistry Fuzhou UniversityFuzhou 350108China state key laboratory of physical chemistry of solid surfaces MOE Key Laboratory of Spectrochemical Analysis and InstrumentationiChEMCollege of Chemistry and Chemical EngineeringCollege of MaterialsCollege of EnergyXiamen UniversityXiamen 361005China Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005China Shenzhen Research Institute of Xiamen University Shenzhen 518000China

The composition and evolution of interfacial species play a key role during electrocatalytic *** the structural evolution and intermediate during catalytic process by in situ characterization can shed new light on the electrocatalytic reaction mechanism and develop highly efficient ***,directly probing the interfacial species is extremely difficult for most spectroscopic techniques due to complicated interfacial environment and ultra-low surface ***,electrochemical core-shell nanoparticle enhanced Raman spectroscopy is utilized to probe the composition and evolution processes of interfacial species on Au@Pt,Au@Co,and Au@PtCo core-shell nanoparticle *** spectral evidences of interfacial intermediates including hydroxide radical(OH*),superoxide ion(O_(2)^(−)),as well as metal oxide species are directly captured by in situ Raman spectroscopy,which are further confirmed by the both isotopic experiment and density functional theory *** results provide a mechanistic guideline for the rational design of highly efficient electrocatalysts.

关键词： in situ Raman core-shell nanoparticle PtCo interfacial species composition and evolution

Color center-rich γ-AlOpromotes propane dehydrogenation

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Science China chemistry 2024年

作者： Yu Wang Xiang Wang Mengfei Qiao Qingyuan Wu Kunlong Liu Xiaodong Yi Ruixuan Qin Gang Fu Nanfeng Zheng state key laboratory for physical chemistry of solid surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University key laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Material SciencesZhejiang Normal University Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM)

The PtSn/Al2O3catalyst is commonly used in commercial propane dehydrogenation （PDH） processes,but it faces challenges in the deactivation and periodic regeneration due to metal aggregation and coke deposition at high *** Al3+pentahas been proven to be beneficial for enhancing catalytic stability,bottom-up synthesis protocols usually restrict their ***,a facile post-treatment approach using acetic acid was applied to create color centers （electrons trapped within oxygen vacancies） on γ-Al3+***,the content of Alpentawas enriched to 18.3%.Then,the pre-established PtSn clusters were *** electrons facilitated the formation of ultrafine PtSn nanoparticles （～2 nm）,and the Al3+pentasites prevented the sintering of PtSn by constructing the strong Al3+penta–O–Sn ***,the catalytic durability of the catalyst prepared by conventional impregnation methods was remarkably extended from 186 h for the color center-free sample to 1,000 h using the HAc–*** facile post-modification was further successfully extended to commercial Al2O3pellets without altering their mechanical properties,highlighting its potential in industrial applications.

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Dynamic tracking of exsolved PdPt alloy/perovskite catalyst for efficient lean methane oxidation

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Chinese Chemical Letters 2024年第4期35卷 170-175页

作者： Yanling Yang Zhenfa Ding Huimin Wang Jianhui Li Yanping Zheng Hongquan Guo Li Zhang Bing Yang Qingqing Gu Haifeng Xiong Yifei Sun College of Energy Xiamen UniversityXiamen 361005China School of Environment and Civil Engineering Dongguan University of TechnologyDongguan 523808China department of chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China CAS key laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China

Supported Pd based catalysts are considered as the efficient candidates for low-carbon alkane oxidation for their outstanding capability to break C-H bond. Whereas, the irreversible deactivation of Pd based catalysts was still frequently observed. Herein, we reinforced the extruded Pd nanoparticles with quantitive Pt to assemble the evenly distributed Pd Pt nanoalloy onto ferrite perovskite(Pd Pt-LCF) matrix with strengthened robustness of metal/oxide support interface. We further co-achieved the enhanced performance, anti-overoxidation as well as resistance of vapor-poisoning in durability measurement. The operando X-ray photoelectron spectroscopy(O-XPS) combined with various morphology characterizations confirms that the accumulation of surface deep-oxidation species of Pd^(4+) is the culprit for fast activity loss in exsolved Pd system, especially at high temperature of 400 ℃. Conversely, it could be completely suppressed by in-situ alloying Pd with equal amount of Pt, which helps maintain the metastable Pd^(2+)/Pd shell and metallic solid-solution core structure. The density function theory(DFT) calculations further buttress that the dissociation of C–H was facilitated on alloy/perovskite interface which is, on the contrary, resistant toward O–H bond cleavage, as compared to Pd/perovskite. Our work suggests that the modification of exsolved metal/oxide catalytic interface could further enrich the toolkit of heterogeneous catalyst design.

关键词： Exsolution PdPt alloy Operando characterization Methane conversion Deep-oxidation

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The proximity between hydroxyl and single atom determines the catalytic reactivity of Rh1/CeO_(2) single-atom catalysts

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Nano Research 2024年第1期17卷 397-406页

作者： Danfeng Wu Shuyun Zhou Congcong Du Juan Li Jianyu Huang Hong-xia Shen Abhaya K.Datye Shan Jiang Jeffrey T.Miller Sen Lin Haifeng Xiong state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China state key laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhou 350002China Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066004China College of Biology and Chemical Engineering Jiaxing UniversityJiaxing 314000China department of Chemical&Biological Engineering University of New MexicoAlbuquerqueNM 8731-0001USA Davidson School of Chemical Engineering Purdue UniversityWest LafayetteIN 47907-2100USA Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China Fujian key laboratory of Rare-earth Functional Materials Fujian Shanhai Collaborative Innovation Center of Rare-earth Functional MaterialsLongyan 366300China

The local structure of the metal single-atom site is closely related to the catalytic activity of metal single-atom catalysts(SACs).However,constructing SACs with homogeneous metal active sites is a challenge due to the surface heterogeneity of the conventional ***,we prepared two Rh1/CeO_(2)SACs(0.5Rh1/r-CeO_(2)and 0.5Rh1/c-CeO_(2),respectively)using two shaped CeO_(2)(rod and cube)exposing different facets,i.e.,CeO_(2)(111)and CeO_(2)(100).In CO oxidation reaction,the T100 of 0.5Rh1/r-CeO_(2)SACs is 120°C,while the T100 of 0.5Rh1/c-CeO_(2)SACs is as high as 200°*** in-situ CO diffuse reflectance infrared Fourier transform spectroscopy(CO-DRIFTS),we found that the proximity between OH group and Rh single atom on the plane surface plays an important role in the catalytic activity of Rh1/CeO_(2)SAC system in CO *** Rh single atom trapped at the CeO_(2)(111)crystal surface forms the Rh1(OH)adjacent species,which is not found on the CeO_(2)(100)crystal surface at room ***,during CO oxidation,the OH group far from Rh single atom on the 0.5Rh1/c-CeO_(2)disappears and forms Rh1(OH)adjacent species when the temperature is above 150°*** formation of Rh1(OH)adjacentCO intermediate in the reaction is pivotal for the excellent catalytic activity,which explains the difference in the catalytic activity of Rh single atoms on two different CeO_(2)*** formed Rh1(OH)adjacent-O-Ce structure exhibits good stability in the reducing atmosphere,maintaining the Rh atomic dispersion after CO oxidation even when pre-reduced at high temperature of 500°*** functional theory(DFT)calculations validate the unique activity and reaction path of the intermediate Rh1(OH)adjacentCO species *** work demonstrates that the proximity between metal single atom and hydroxyl can determine the formation of active intermediates to affect the catalytic performances in catalysis.

关键词： crystal plane Rh1/CeO_(2)single-atom catalyst proximity of Rh and hydroxyl coordination structure CO oxidation