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“Buckets effect”in the kinetics of electrocatalytic reactions

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Journal of Energy Chemistry 2024年第2期89卷 388-396,I0010页

作者： Haowen Cui Yan-Xia Chen hefei national laboratory for physical sciences at Microscale Department of Chemical PhysicsUniversity of Science and Technology of ChinaHefei 230026AnhuiChina

In this study,we systematically investigated the effect of proton concentration on the kinetics of the oxygen reduction reaction(ORR)on Pt(111)in acidic solutions.Experimental results demonstrate a rectangular hyperbolic relationship,i.e.,the ORR current excluding the effect of other variables increases with proton concentration and then tends to a constant value.We consider that this is caused by the limitation of ORR kinetics by the trace oxygen concentration in the solution,which determines the upper limit of ORR kinetics.A model of effective concentration is further proposed for rectangular hyperbolic relationships:when the reactant concentration is high enough to reach a critical saturation concentration,the effective reactant concentration will become a constant value.This could be due to the limited concentration of a certain reactant for reactions involving more than one reactant or the limited number of active sites available on the catalyst.Our study provides new insights into the kinetics of electrocatalytic reactions,and it is important for the proper evaluation of catalyst activity and the study of structureperformance relationships.

关键词： Oxygen reduction reaction Kinetics Zero order Rectangular hyperbolic relationship pH effect

Advances in bio-inspired electrocatalysts for clean energy future

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Nano Research 2024年第2期17卷 515-533页

作者： Jing-Wen Duan Mu Min-Rui Gao Division of Nanomaterials&Chemistry Hefei National Laboratory for Physical Sciences at the MicroscaleDepartment of ChemistryUniversity of Science and Technology of ChinaHefei 230026China

Electrocatalysis can enable efficient energy storage and conversion and thus is an effective way to achieve carbon neutrality.The unique structure and function of organisms can offer many ideas for the design of electrocatalysts,which has become one of the most promising research directions.Recently,the understanding of the mechanism of bio-inspired electrocatalysis has become clearer,which has promoted the design of bio-inspired catalysts and catalytic systems.Various bio-inspired catalysts(enzyme-like catalysts,layered porous catalysts,superhydrophobic/superhydrophilic surfaces,and so on)have been developed to enable efficient electrocatalytic reactions.Herein,we discuss the key advances in the field of bio-inspired electrocatalysts progressed in recent years.First,the role of bio-inspiration in increasing the intrinsic activity and number of active sites of catalysts is introduced.Then,the structure and mechanism of layered porous catalytic systems that mimic biological transport systems are comprehensively discussed.Subsequently,the design of three-phase interfaces from micro-nanoscale to atomic scale is highlighted,including the wettability of the electrode surface and the transport system near the electrode.We conclude the review by identifying challenges in bio-inspired electrocatalysts and providing insights into future prospects for the exciting research field.

关键词： bio-inspired electrocatalysts active sites layered porous structure three-phase interface

Experimental Proposal on Non-Hermitian Skin Effect by Two-dimensional Quantum Walk with a Single Trapped Ion

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Chinese Physics Letters 2024年第4期41卷 19-24页

作者：侯琬儿唐皓许勤林毅恒 CAS Key laboratory of Microscale Magnetic Resonance and School of physical sciences University of Science and Technology of ChinaHefei 230026China hefei national laboratory University of Science and Technology of ChinaHefei 230088China

Non-Hermitian Hamiltonians are widely used in describing open systems with gain and loss,among which a key phenomenon is the non-Hermitian skin effect.Here we report an experimental scheme to realize a twodimensional(2D)discrete-time quantum walk with non-Hermitian skin effect in a single trapped ion.It is shown that the coin and 2D walker states can be labeled in the spin of the ion and the coherent-state lattice of the ion motion,respectively.We numerically observe a directional bulk flow,whose orientations are controlled by dissipative parameters,showing the emergence of the non-Hermitian skin effect.We then discuss an experimental implementation of our scheme in a laser-controlled trapped Ca^(+)ion.Our experimental proposal may be applicable to research of dissipative quantum walk systems and may be able to generalize to other platforms,such as superconducting circuits and atoms in cavity.

关键词： effect dissipative quantum

Topological and superconducting properties of monolayered CoN and CoP:A first-principles comparative study

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Science China(Physics,Mechanics & Astronomy) 2024年第5期67卷 98-108页

作者： Jiaqing Gao Zhenyu Zhang Ping Cui International Center for Quantum Design of Functional Materials(ICQD) Hefei National Research Center for Physical Sciences at Microscale(HFNL)University of Science and Technology of ChinaHefei 230026China hefei national laboratory University of Science and Technology of ChinaHefei 230088China

Two-dimensional systems that simultaneously harbor superconductivity and nontrivial band topology may serve as appealing platforms for realizing topological superconductivity with promising applications in fault-tolerant quantum computing.Here,based on first-principles calculations,we show that monolayered Co N and Co P with the isovalent Fe Se-like structure are stable in freestanding form,even though their known bulk phases have no resemblance to layering.The two systems are further revealed to display intrinsic band inversions due to crystal field splitting,and such orderings are preserved with the inclusion of spin-orbit coupling(SOC),which otherwise is able to open a curved band gap,yielding a non-zero Z2 topological invariant in each case.Such a mechanism of topologicalization is distinctly contrasted with that identified recently for the closely related monolayers of CoX(X=As,Sb,Bi),where the SOC plays an indispensable role in causing a nontrivial band inversion.Next,we demonstrate that,by applying equi-biaxial tensile strain,the electron-phonon coupling strength in monolayered CoN can be significantly enhanced,yielding a superconducting transition temperature(Tc)up to 7-12 K for the Coulomb pseudopotential ofμ*=0.2-0.1,while the CoP monolayer shows very low Tc even under pronounced strain.Their different superconducting behaviors can be attributed to different variations in lattice softening and electronic density of states around the Fermi level upon pressuring.Our central findings enrich the understanding of different mechanisms of band inversions and topologicalization and offer platforms for achieving the coexistence of superconductivity and nontrivial band topology based on two-dimensional systems.

关键词： topological yielding otherwise

High-rate CH_(4)-to-C_(2)H_(6) photoconversion enabled by Au/ZnO porous nanosheets under oxygen-free system

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Science China Chemistry 2024年第3期67卷 869-875页

作者： Kai Zheng Xiaojing Zhang Jun Hu Chengbin Xu Juncheng Zhu Jing Li Mingyu Wu Shan Zhu Li Li Shumin Wang Yumei Lv Xin He Ming Zuo Chengyuan Liu Yang Pan Junfa Zhu Yongfu Sun Yi Xie hefei national laboratory for physical sciences at Microscale National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China Key laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China State Grid Anhui Electric Power Research Institute Hefei 230601China

Photocatalytic CH_(4) coupling into high-valued C_(2)H_(6) is highly attractive,whereas the photosynthetic rate,especially under oxygen-free system,is still unsatisfying.Here,we designed the negatively charged metal supported on metal oxide nanosheets to activate the inert C-H bond in CH_(4)and hence accelerate CH_(4) coupling performance.As an example,the synthetic Au/ZnO porous nanosheets exhibit the C_(2)H_(6) photosynthetic rate of 1,121.6μmol g^(-1)_(cat)h^(-1)and the CH_(4) conversion rate of 2,374.6μmol g^(-1)_(cat)h^(-1) under oxygen-free system,2 orders of magnitude higher than those of previously reported photocatalysts.By virtue of several in situ spectroscopic techniques,it is established that the generated Au^(δ-)and O^-species together polarized the C-H bond,while the Au^(δ-)and O^-species jointly stabilized the CH_(3) intermediates,which favored the coupling of CH_(3) intermediate to photosynthesize C_(2)H_(6) instead of overoxidation into CO_(x).Thus,the design of dual active species is beneficial for achieving high-efficient CH_(4)-to-C_(2)H_(6) photoconversion.

关键词： dual surface-active sites selective methane coupling ethane room temperature

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 conversion.Herein,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 wastes.During the carbonization,zinc salts are thermally decomposed into nanoparticles that serve as in-situ templates to introduce nanopores in carbons.The 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 distributions.Moreover,the zinc salts can be recovered and recycled,supporting the sustainable production of HPCs on large scale.The 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

Regulating atomic Fe-Rh site distance for efficient oxygen reduction reaction

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Science China Chemistry 2024年第4期67卷 1352-1359页

作者： Tong Liu Yudan Chen Airong Xu Xiaokang Liu Dong Liu Sicheng Li Hui Huang Li Xu Shuaiwei Jiang Qiquan Luo Tao Ding Tao Yao national Synchrotron Radiation laboratory University of Science and Technology of ChinaHefei 230029China Key laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefei 230026China Institutes of physical Science and Information Technology Anhui UniversityHefei 230601China

Exploring the atomic interaction mechanisms of dense single-atom catalysts(SACs)is of great significance for their application in oxygen reduction reaction(ORR).However,the intrinsic mechanism of the site-distance effect on the catalytic performance has been largely ignored.Here,we demonstrate the site-distance effect of Fe-Rh_(x)@NC catalysts in ORR theoretically and experimentally.Bader charge analysis reveals that the strong interaction between Fe and Rh atoms at a certain atomic distance(dFe-Rh)alters the catalytic electronic structure,facilitating the optimization of catalyst adsorption strength.Motivated by the theoretical calculations,we designed and synthesized the Fe-Rhx@NC catalysts through a spatial confinement strategy.The characterization results prove that the Fe-Rh_(2)@NC has the optimal d_(Fe-Rh),which improves its intrinsic ORR activity,providing a half wave potential of 0.91 V,higher than that of the commercial Pt/C(0.86 V).This study emphasizes the importance of determining the basic mechanism of the site-distance effect in dissimilar metal atoms catalysts,which is conducive to the design of efficient catalyst systems for practical applications.

关键词： Density functional theory single-atom catalyst in-situ encapsulating site-distance effect oxygen reduction reaction

Overcoming the Na-ion conductivity bottleneck for the cost-competitive chloride solid electrolytes

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Journal of Energy Chemistry 2024年第8期95卷 1-8页

作者： Lv Hu Hui Li Fang Chen Yating Liu Jinzhu Wang Cheng Ma hefei national Research Center for physical sciences at the Microscale CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering University of Science and Technology of China national Synchrotron Radiation laboratory

Chloride solid electrolytes possess multiple advantages for the construction of safe,energy-dense allsolid-state sodium batteries,but presently the chlorides with sufficiently high cost-competitiveness for commercialization almost all exhibit low Na-ion conductivities of around 10-5S cm-1or lower.Here,we report a chloride solid electrolyte,Na2.7ZFCl5.3O0.7,which reaches a Na-ion conductivity of2.29 × 10-4S cm-1at 25℃ without involving overly expensive raw materials such as rare-earth chlorides or Na2S.In addition to the efficient ion transport,Na2.7ZrCl5.3O0.7also shows an excellent deformability surpassing that of the widely studied Na3PS4,Na3SbS4,and Na2ZrCl6solid electrolytes.The combination of these advantages allows the all-solid-state cell based on Na2.7ZrCl5.3O0.7and NaCrO2to realize stable room-temperature cycling at a much higher specific current than those based on other non-viscoelastic chloride solid electrolytes in literature(120 mA g-1vs.12-55 mA g-1);after 100 cycles at such a high rate,the Na2.7ZFCl5.3O0.7-based cell can still deliver a discharge capacity of 80 mAh g-1at25℃.

关键词： All-solid-state sodium batteries Chlorides High voltage stability Ionic conductivities Solid electrolytes

Efficient synthesis of bottle-brush polymers enabled by selective photoactivation strategy in NIR-induced PET-RAFT polymerization

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Science China Chemistry 2024年第7期67卷 2353-2361页

作者： Hao Zha Lin Cheng 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

Bottle-brush polymers possessing densely grafted side chains have special properties that are distinct from linear macromolecules.Herein,an efficient method for preparing bottle-brush polymers based on a selective photoactivation strategy in the photoinduced electron/energy transfer reversible addition-fragmentation chain transfer(PET-RAFT)polymerization was developed.A methacrylate monomer 2-(2-(dodecylthiocarbonothioylthio)propionate)ethyl methacrylate(DTPEMA)containing a 2-(dodecylthiocarbonothioylthio)propionate(DTP)unit with a secondary R group was designed.Utilizing the unique selectivity of metal naphthalocyanine photocatalyst zinc 2,11,20,29-tetra-tert-butyl-2,3-naphthalocyanine(ZnTtBNc)toward trithiocarbonate with tertiary R group,the PET-RAFT polymerization of DTPEMA catalyzed by ZnTtBNc was performed under near infrared(NIR)light(λ_(max)=760 nm)irradiation at room temperature,using 4-cyano-4-[(dodecylsulfanylthiocarbonyl)-sulfanyl]pentanoic acid(CDTPA)with a tertiary R group as a chain transfer agent(CTA).Proton nuclear magnetic resonance(1H NMR)and gel permeation chromatography(GPC)results demonstrated that the DTP units in the side chains were inert during the polymerization.By grafting poly(methyl acrylate)(PMA)from PDTPEMA via thermal-initiated RAFT polymerization,welldefined P(DTPEMA-g-PMA)bottle-brush polymers could be afforded.Furthermore,the film prepared from the bottle-brush polymer exhibited excellent scratch self-healing property due to the interlocking of side chains.

关键词： bottle-brush polymers PET-RAFT polymerization selective photoactivation scratch self-healing