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Deciphering the linear relationship in the activity of the oxygen reduction reaction on Pt electrodes:A decisive role of adsorbates

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Journal of Energy Chemistry 2024年第7期94卷 70-77页

作者： Haowen Cui Yan-Xia Chen hefei national Research Center for physical sciences at microscale and department of chemical physics University of Science and Technology of ChinaHefei 230026AnhuiChina

Despite substantial efforts in developing high-performance catalysts for the oxygen reduction reaction(ORR),the persistent challenge lies in the high onset overpotential of the ORR,and the effect of the elec-trolyte solution cannot be ***,we have systematically investigated the impact of adsorbate species and concentration,as well as solution pH,on the ORR activity on Pt(111)and Pt(poly)*** results all tend to establish a linear quantitative relationship between the onset potential for ORR and the adsorption equilibrium potential of the *** finding indicates the decisive role of adsorbates in the onset potential for ORR,suggesting that the adsorption potential of adsorbates can serve as an intuitive criterion for ORR *** support for this conclusion is derived from experimental results obtained from the oxygen evolution reaction on Pt(poly)with different adsorbate species and from the hydrogen evolution reaction on Pt(111)with iodine *** further propose both an empirical equation for the onset potential for ORR and the concept of a potential-regulated adsor-bate shielding effect to elucidate the influence of adsorbates on ORR *** study provides new insights into the high onset overpotential of the ORR and offers potential strategies for predicting and enhancingORRactivity inthefuture.

关键词： Oxygen reduction reaction Activity Adsorbate Equilibrium potential Pt(111)

Holevo bound independent of weight matrices for estimating two parameters of a qubit

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Chinese physics B 2024年第2期33卷 137-143页

作者：牛畅郁司夏 department of Modern physics&hefei national Research Center for physical sciences at the microscale and School of physical sciences University of Science and Technology of ChinaHefei 230026China hefei national laboratory University of Science and Technology of ChinaHefei 230088China

Holevo bound plays an important role in quantum metrology as it sets the ultimate limit for multi-parameter estimations,which can be asymptotically *** for some trivial cases,the Holevo bound is implicitly defined and formulated with the help of weight *** we report the first instance of an intrinsic Holevo bound,namely,without any reference to weight matrices,in a nontrivial ***,we prove that the Holevo bound for estimating two parameters of a qubit is equivalent to the joint constraint imposed by two quantum Cramér–Rao bounds corresponding to symmetric and right logarithmic *** weightless form of Holevo bound enables us to determine the precise range of independent entries of the mean-square error matrix,i.e.,two variances and one covariance that quantify the precisions of the estimation,as illustrated by different estimation *** result sheds some new light on the relations between the Holevo bound and quantum Cramer–Rao *** generalizations are discussed.

关键词： quantum metrology quantum Fisher information Holevo bound quantum multi-parameter estimation

Dynamic kinetic stereodivergent transformations of propargylic ammonium salts via dual nickel and copper catalysis

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Chinese chemical Letters 2024年第8期35卷 265-269页

作者： Ruilong Geng Lingzi Peng Chang Guo hefei national laboratory for physical sciences at the microscale and department of Chemistry University of Science and Technology of ChinaHefei 230026China

The dynamic kinetic asymmetric transformation of racemic propargylic ammonium salts with prochiral aldimine esters through a stereodivergent propargylation is catalyzed by dual nickel and copper ***,a diverse range of optically activeα-quaternary amino esters were produced via C-N bond cleavage with high reaction efficiency and stereoselectivity(up to>99%ee).By selection of the appropriate pair-wise combination of catalyst configurational isomers,all four possible stereoisomers of the corresponding propargylation products are obtained in high yields with excellent regio-,diastereo-,and enantioselectiv-ities.

关键词： Stereodivergent propargylation Dual catalysis C-N bond cleavage Azaomethine ylides Internal propargylic ammonium salts Excellent stereoselectivity

Synthesis of hierarchically porous carbon materials by zinc salts-assisted carbonization of biomass and organic solid wastes

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Particuology 2024年第1期84卷 45-52页

作者： Le-Le Zhang Lei Tong Yanwei Ding Wanqun Zhang Hai-Wei Liang hefei national Research Center for physical sciences at the microscale Department of ChemistryUniversity of Science and Technology of ChinaHefei230026China

Hierarchically porous carbons(HPCs)with multimodal pores have attracted considerable attention due to their unique physical and chemical properties and various application potentials in heterogeneous catalysis,environmental treatment,and energy storage and ***,we report a general and simple zinc salts-assisted method for the synthesis of HPCs with varied porosity and chemical func-tionalities by the direct carbonization of diverse biomass and *** the carbonization,zinc salts are thermally decomposed into nanoparticles that serve as in-situ templates to introduce nanopores in *** prepared HPCs exhibit high specific surface areas(up to 2432 m2 g-1),large pore volumes(up to 4.30 cm^(3)g^(-1)),and broad pore size ***,the zinc salts can be recovered and recycled,supporting the sustainable production of HPCs on large *** prepared HPCs-supported catalysts with atomically dispersed metal sites exhibit promising electrocatalytic performance for the oxygen reduction reaction.

关键词： Hierarchical porous carbon Zinc salts Biomass Wastes Electrocatalysis

Surface evolution of thermoelectric material KCu_(4)Se_(3) explored by scanning tunneling microscopy

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Chinese physics B 2024年第8期33卷 422-427页

作者：夏玉敏马妮蔡德胜刘宇舟谷易通于淦霍思宇庞文慧肖翀秦胜勇 International Center for Quantum Design of Functional Materials(ICQD) Hefei National Laboratory for Physical Sciences at Microscale(HFNL)University of Science and Technology of ChinaHefei 230026China CAS Key laboratory of Strong Coupled Quantum Matter physics Department of PhysicsUniversity of Science and Technology of ChinaHefei 230026China hefei national laboratory for physical sciences at the microscale University of Science and Technology of ChinaHefei 230026China Institute of Energy Hefei Comprehensive National Science CenterHefei 230031China Dalian national laboratory for Clean Energy Chinese Academy of Sciences(CAS)Dalian 116023China hefei national laboratory University of Science and Technology of ChinaHefei 230088China

Novel two-dimensional thermoelectric materials have attracted significant attention in the field of thermoelectric due to their low lattice thermal conductivity.A comprehensive understanding of their microscopic structures is crucial for driving further the optimization of materials properties and developing novel functional ***,by using in situ scanning tunneling microscopy,we report the atomic layer evolution and surface reconstruction on the cleaved thermoelectric material KCu_(4)Se_(3) for the first *** clearly revealed each atomic layer,including the naturally cleaved K atomic layer,the intermediate Se^(2-)atomic layer,and the Se^(-)atomic layer that emerges in the thermodynamic-stable *** from the maj ority of studies that predominantly concentrate on macroscopic measurements of the charge transport,our results reveal the coexistence of potassium disorder and complex reconstructed patterns of selenium,which potentially influences charge carrier and lattice *** results provide direct insight into the surface microstructures and evolution of KCu_(4)Se_(3),and shed useful light on designing functional materials with superior performance.

关键词： thermoelectric KCu_(4)Se_(3) scanning tunneling microscopy(STM) evolution

Room-temperature ferrimagnetism and size-modulated electronic structures in two-dimensional cluster-based metal-organic frameworks

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Science China Chemistry 2024年第4期67卷 1334-1340页

作者： Jing Cheng Xingxing Li Jinlong Yang Key laboratory of Precision and Intelligent Chemistry University of Science and Technology of ChinaHefei 230026China department of chemical physics University of Science and Technology of ChinaHefei 230026China hefei national Research Center for physical sciences at the microscale University of Science and Technology of ChinaHefei 230026China hefei national laboratory University of Science and Technology of ChinaHefei 230088China

Cluster-assembled materials have attracted particular attention for their complex hierarchical structures and unique ***,the majority of cluster-based assemblies developed so far are either non-magnetic or only exhibit magnetic ordering with a relatively low Curie temperature,limiting their applications in ***,two-dimensional(2D)cluster-assembled materials with room-temperature magnetism remain highly *** this purpose,based on first principles calculations,we design a series of thermodynamically stable 2D cluster-based metal-organic frameworks(MOFs)Fe_(n)-(pyz)(n=1-6)by utilizing Fenmetal clusters as nodes and nitrogen-containing pyrazine ligands as organic *** 2D cluster-based MOFs exhibit robust ferrimagnetic ordering due to the strong d-p direct exchange interaction between d-electron spin of Fe_(n)(n=1-6)clusters and charge transfer-induced p-electron spin of pyrazine *** particular,the ferrimagnetic Curie temperatures are well above room temperature(up to 836 K).Additionally,altering the size of Fe_(n)clusters in Fe_(n)-(pyz)(n=1-6)MOFs results in diverse functional spintronic properties,including bipolar magnetic semiconductors,half semiconductors and Dirac half ***,these 2D assembled MOFs possess sizable magnetic anisotropy energies,up to 9.16 me V per formula.

关键词： metal-organic framework two-dimensional material half metal bipolar magnetic semiconductor magnet

Alloy strategy to synthesize Pt-early transition metal oxide interfacial catalysts

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Nano Research 2024年第4期17卷 3390-3397页

作者： Shi-Long Xu Hang Nan Wanqun Zhang Yue Lin Sheng-Qi Chu Hai-Wei Liang hefei national Research Center for physical sciences at the microscale Department of ChemistryUniversity of Science and Technology of ChinaHefei 230026China School of Materials and chemical Engineering Anhui Jianzhu UniversityHefei 230601China Institute of High Energy physics Chinese Academy of SciencesBeijing 100049China

Metal oxide supported metal catalysts show promising catalytic performance in many industry-relevant ***,the enhancement of performance is often limited by the insufficient metal/metal oxide *** this work,we demonstrate a general synthesis of Pt-early transition metal oxide(Pt-MO_(x),M=Ti,Zr,V,and Y)catalysts with rich interfacial sites,which is based on the air-induced surface segregation and oxidation of M in the supported Pt-M alloy *** characterizations verify the dynamic structural response of Pt-M alloy catalysts to air and the formation of Pt-MO_(x) catalysts with abundant interfacial *** prepared Pt-TiO_(x) interfacial catalysts exhibit improved performance in hydrogenation reactions of benzaldehyde,nitrobenzene,styrene,and furfural,as a result of the heterolytic dissociation of H_(2) at Pt-metal oxide interfacial sites.

关键词： Pt-early transition metal oxide interfacial catalyst alloy oxidation strategy interfacial sites hydrogenation reactions heterolytic dissociation

Preparing cyclic polymers at high concentrations via self-folding cyclization technique by adjusting the contents of hydrophilic units in linear precursors

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Chinese chemical Letters 2024年第2期35卷 283-288页

作者： Hao Zha Zuowei Wang Chao Liu Chunyan Hong department of Polymer Science and Engineering University of Science and Technology of ChinaHefei 230026China hefei national laboratory for physical sciences at the microscale University of Science and Technology of ChinaHefei 230026China

Cyclic polymers are a class of polymers that feature endless topology,and the synthesis of cyclic polymers has attracted the attention of many ***,cyclic polymers were efficiently constructed by self-folding cyclization technique at high *** poly((oligo(ethylene glycol)acrylate)-co-(dodecyl acrylate))(P(OEGA-co-DDA))precursors with different ratios of hydrophilic and hydrophobic moieties were synthesized by reversible addition-fragmentation chain transfer(RAFT)polymerization using a bifunctional chain transfer agent with two anthryl end *** amphiphilic linear precursors underwent the self-folding process to generate polymeric nanoparticles in *** irradiating the aqueous solution of the nanoparticles with 365 nm UV light,cyclic polymers were synthesized successfully via coupling of anthryl *** effects of the ratios of hydrophilic and hydrophobic moieties in linear P(OEGA-co-DDA)copolymers and polymer concentration on the purity of the obtained cyclic polymers were explored in detail via ^(1)H nuclear magnetic resonance(^(1)H NMR),dynamic light scattering(DLS),UV‒visible(vis)analysis,three-detection size exclusion chromatography(TD-SEC)and transmission electron microscopy(TEM).It was found that by adjusting the content of the hydrophilic segments in linear precursors,single chain polymeric nanoparticles(SCPNs)can be generated at high polymer ***,cyclic polymers with high purity can be constructed *** method overcomes the limitation of traditional ring-closure method,which is typically conducted in highly dilute conditions,providing an efficient method for the scalable preparation of cyclic polymers.

关键词： Cyclic polymers Self-folding cyclization technique Single chain polymeric nanoparticles RAFT polymerization Direct visualization

Double stimulus-responsive palladium catalysts for ethylene polymerization and copolymerization

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Chinese chemical Letters 2024年第7期35卷 407-411页

作者： Hailong He Wenbing Wang Wenmin Pang Chen Zou Dan Peng CAS Key laboratory of Soft Matter Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei National Laboratory for Physical Sciences at the MicroscaleHefei 230026China

The external stimulus response strategy has been evolved rapidly in the field of olefin *** this work,we modularly synthesized three types of double stimulus responsiveα-diimine palladium catalysts,combining redox regulation and other regulation together,such as light,Lewis acid and alkali *** catalytic activities and the molecular weight of polyethylene products can be regulated for 4 times in ethylene *** palladium complexes were also used for the copolymerization reaction of ethylene and polar monomers,such as methyl 10-undecylenate and methyl acrylate,effectively regulating the catalytic activities,the molecular weight and polar monomer incorporation of the prepared *** research on these dual-regulated palladium complexes makes full use of prepared catalysts and provides new inspirations for regulating olefin polymerization.

关键词： Dual-regulated Stimulus-responsive Palladium Ethylene polymerization Polar monomer