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Cathodic corrosion as a facile and universal method for scalable preparation of dual-atom electrocatalysts

Nano Research 2025年第4期18卷 70-77页

作者： Rui Li Tao Shao Fudong Jiang Dong Chen Wenyong Jing Jingwen Ba Yulong Li Yuhan Wu Wenhua Luo Jingsong Xu Institute of Materials China Academy of Engineering PhysicsMianyang 621907China Science and Technology on Surface Physics and Chemistry Laboratory Mianyang 621908China

Dual-atom catalysts(DACs)are emerging as highly efficient electrocatalysts,offering synergistic effects and high atomic ***,we introduce a scalable and facile electrochemical approach for the top-down synthesis of DACs supported on carbon materials via a two-time“plasma treatment+cathodic corrosion”***,metal atoms in nanoparticles on cathode are etched under high negative potential,diffused over the electrode,captured by N doped carbon carriers in electrolyte and forming single-atom *** introducing additional N coordination sites adjacent to the primary metal single-atom sites via a secondary plasma processing and anchoring a second metal atom via a subsequent cathodic corrosion process,DACs are *** as-prepared Pt DACs exhibit enhanced catalytic activity toward hydrogen evolution reaction(HER)with a low overpotential of 0.027 V at 10 mA·cm^(-2) and a Tafel slope of 29.9 mV·dec^(-1) as well as high ***,the proposed electrochemical top-down synthetic route affords promising potential for scalable production of other homonuclear or heteronuclear DACs on multiple carbon substrates,advancing the practical application of DACs in electrocatalysis.

关键词： dual-atom catalysts cathodic corrosion top-down strategy scalable synthesis hydrogen evolution reaction

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CO adsorption, activation, and oxidation on CeO_(2)(111)-supported Fe model catalyst surfaces

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Nano Research 2025年第2期18卷 111-119页

作者： Xingwang Cheng Yi Tu Dongling Zhang Dong Han Luchao Huang Jun Hu Honghe Ding Qian Xu Junfa Zhu National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Department of Chemical Physics Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutesand Key Laboratory of Precision and Intelligent ChemistryUniversity of Science and Technology of ChinaHefei 230026China

Elucidating the synergistic effect of Fe on CeO_(2) is challenging in CO-related reactions but attractive owing to the improvement in the oxygen storage/release capacity of ceria with the addition of ***,using CeO_(2)(111)-supported Fe model catalysts,CO adsorption,activation,and oxidation on catalyst surfaces was carefully investigated using synchrotron radiation photoemission spectroscopy(SRPES),temperature-programmed desorption(TPD),and infrared reflection absorption spectroscopy(IRRAS).The precursorπ-bonding state for CO dissociative adsorption has been identified through unusually low CO vibration frequencies and a low 0 ML 0.6 ML Top sites Bridge sites MS intensity 1.0 MLπ-bond state 2.0 ML Fe 3p hv=180 eV 100 L CO on 1.6 ML Fe/CeO_(2)(111)54.7 eV Fe^(2+)53.3 eV Fe 01142 cm−1 Recombination desorption Intensity(a.u.)Clean 100 L 150 K 200 K 250 K 300 K 400 K 600 K 100200300400500600700 Temperature(K)6058565452 Binding energy(eV)50 dissociation temperature on Fe/CeO_(2)(111)*** is oxidized by dissociated atomic O followed by the Langmuir–Hinshelwood mechanism,whereas the lattice oxygen of CeO_(2) exhibits low *** CO_(2) yield displays a volcanic curve as a function of Fe *** the 0.6 ML Fe/CeO_(2) surface,weakly bound atomic O on Fe^(2+)results in the best catalytic *** on high Fe coverage surfaces,the CO_(2) yield is limited due to the capture of atomic O by *** results provide comprehensive insights into the adsorption,activation,and oxidation of CO on Fe/CeO_(2) and identify the reaction mechanism,and the active site,which provides deeper insights into CO-related reaction mechanisms over CeO_(2) supported Fe catalysts.

关键词： iron/ceria model catalyst adsorption activation oxidation

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Strain-induced Stereocomplex Formation from the Initially Amorphous Poly(L-lactic acid)/Poly(D-lactic acid) Samples

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Chinese Journal of Polymer science 2025年第4期43卷 655-665页

作者： Tao Liao Zhi-yong Jiang Yong-feng Men State Key Laboratory of Polymer Physics and Chemistry&Key Laboratory of Polymer Science and Technology Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The strain-induced crystallization behaviors of ultrasonic micro-injection molded poly(L-lactic acid)/poly(D-lactic acid)(PLLA/PDLA)samples from an amorphous state were investigated by stress-strain relations and in situ wide angle X-ray diffraction(WAXD) *** formation of direct strain-induced stereocomplex(SC) was *** samples molded at 50 and 80℃,this phenomenon can be attributed to the acceleration of the ordered structures due to the existence of a large number of SC *** SC nuclei are assumed to serve as the transient physical cross-links to initiate the strain-induced *** onset of strain-induced crystallization is analogous to the heating induced structural ***,the observed strain-induced SC process can be considered a pseudo process,which is actually thermally *** further stretching,the actual strain-induced crystallization occurs with the exclusive formation of the homocrystallite(HC),while the preceding formed SC crystals undergo slight fragmentation during subsequent tensile *** 120 ℃,due to the reduced number of SC nuclei within the sample,the occurrence of cold crystallization during stretching plays a more significant role than SC nuclei with respect to the strain-induced SC process,as demonstrated by in situ WAXD measurements upon annealing in both the static and stretched states.

关键词： Amorphous PLLA/PDLA blend Strain-induced crystallization Strain-induced SC formation

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Investigation of surface effect in amorphous catalytic active layer for boosted water and seawater oxidation

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Journal of Energy chemistry 2025年第4期103卷 393-399页

作者： Xueqing Gao Yu Zhu Shujiao Yang Wei Zhang Rui Cao College of Chemical and Pharmaceutical Engineering Hebei University of Science and Technology Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education School of Chemistry and Chemical Engineering Shaanxi Normal University

Understanding the catalytic mechanism at real catalytically active layer is essential for the advancement of water ***,it is difficult to explore the surface effect of active layer of catalysts on oxygen evolution reaction（OER） independently because of the coexistence of bulk phase and surfaceactive ***,by designing ultra-thin shell amorphous CoOxhollow nanospheres,we explored the effect of single catalytic active layer on OER activity,further revealing the surface catalytic mechanism for seawater *** amorphous catalytic active layer CoOxcontain phosphates（CoOxPO4）,induced by completely bulk reconstruction of CoPxhollow *** with autologous crystalline CoO,amorphous catalytic active species CoOx-PO4possesses higher OER performance with ultralow overpotential of 229 mV to achieve 10 mA ***,self-built phosphate film could effectively block chloride anions and implement robust seawater *** work brings direct insights of the surface effect of amorphous catalytic active layer on water oxidation,which is critical for the performance optimization of water oxidation.

关键词： Cobalt phosphide Electrocatalysis Reconstruction Seawater Water oxidation

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Exceptional functionalized dual-acidic ionic liquid: High-efficiency catalytic reaction medium for oxidation desulfurization

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Petroleum science 2025年第1期22卷 492-507页

作者： Ran Liu Chang Wang Qiang Yang Jing-Ran Yang Chen Liu Liberty Mguni Xin-Ying Liu Ya-Li Yao Fa-Tang Li Institute for Catalysis and Energy Solutions University of South Africa International Joint Laboratory of New Energy College of Chemistry and Pharmaceutical Engineering Hebei University of Science and Technology Hebei Key Laboratory of Photoelectric Control on Surface and Interface College of Science Hebei University of Science and Technology

The development of highly active functionalized ionic liquids（ILs） as both extractants and catalysts for use in achieving deep desulfurization continues to pose *** this study,a highly efficient oxidative desulfurization system was constructed,composed of dual-acidic ionic liquids（DILs） and *** investigation results of four DILs prepared from different metal chlorides（[HSO3C3NEt3]ClMnCln,MnCl_n=AlCl3,ZnCl2,CuCl2,FeCl3） in oxidative desulfurization showed that [HSO3C3NEt3]Cl-AlCl3had an outstanding catalytic effect and significantly promoted the oxidation of *** a0.2 g [HSO3C3NEt3]Cl-AlCl3,the removal rate of dibenzothiophene（DBT） reached 100% in 10 mL model oil under mild conditions at 55℃ for 20 *** key is its ability to induce the dismutation of superoxide anions（·O2-）,which facilitates the generation of singlet oxygen（1O2）.The efficient oxidation of DBT is accomplished through a predominantly1O2-mediated non-radical mechanism.[HSO3C3NEt3]ClAlCl3serves as a favorable medium for contact to be made between1O2and sulfides,which indicates an efficient catalytic-adsorption synergy.

关键词： Dual-acidic ionic liquid Catalysis Oxidation desulfurization Reactive oxygen species

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Complementary self-assembled monolayers enabling improved energy level alignment in inverted perovskite solar cells

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Journal of Energy chemistry 2025年第5期104卷 136-145页

作者： Shantao Zhang Xiaofen Jiang Xue Wang Yan Gao Tian Ao Hou Xiaoqian Teng Haolin Wang Wenjing Chen Shuang Gao Xinyu Li Ziqi Hu Xiaojun Wu Zhengguo Xiao Tao Chen Yanwu Zhu Yalin Lu Xiaocheng Zeng Zonglong Zhu Shangfeng Yang Key Laboratory of Precision and Intelligent Chemistry Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) Department of Materials Science and Engineering University of Science and Technology of China Department of Chemistry and Shenzhen Research Institute City University of Hong Kong Department of Physics CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics University of Science and Technology of China Department of Materials Science and Engineering City University of Hong Kong

Self-assembled monolayers(SAMs) have been commonly employed as hole-selective layers(HSLs) in inverted(p-i-n) perovskite solar cells(PSCs), and typically only a single-component SAM is applied,which plays limited role in selective hole transport. Herein, we synthesize a novel SAM,(4-(3,11-dibro mo-7H-dibenzo[c,g]carbazol-7-yl)butyl)phosphonic acid(Br-4PADBC), and apply it as a complementary component to the commonly used [2-(3,6-dimeth oxy-9H-carbazol-9-yl)ethyl]phosphonic acid(MeO-2PACz) SAM, accomplishing boosted hole transport in inverted PSCs. A series of characterizations and theoretical calculations are employed to unravel the roles of each components within the binary SAM(bi-SAM). The involvements of the non-planar dibenzo[c,g]carbazole unit and electron-withdrawing Br atoms induce larger dipole moment of Br-4PADBC than MeO-2PACz, resulting in much deeper work function of ITO and consequently improved alignment with the valence band energy level of ***, the introduced Br atoms improve the quality of perovskite crystals and help passivate defects of perovskite. On the other hand, the existence of the conventional MeO-2PACz SAM ensures the considerable conductivity of the bi-SAM and thus efficient hole extraction from the perovskite layer. As a result,inverted PSC devices based on bi-SAM HSL deliver a decent power conversion efficiency(PCE) of 24.52%as well as dramatically improved thermal and operational stabilities.

关键词： Dibenzo[c,g]carbazole Dipole moment Hole-selective layer Perovskite solar cells Self-assembled monolayer

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Modulation of inactive Li2O via iodinated MOF nanocapsules interfacial transformation engineering for high-performance solid electrolyte interphase

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Journal of Energy chemistry 2025年第5期104卷 482-493页

作者： Xingxing Zhang Qingmei Su Gaohui Du Bingshe Xu Xuehan Hou Xiaowei Yang Weihao Shi Zhuo Chen Yang Shi Yujie Lv Wenhuan Huang School of Materials Science & Engineering Shaanxi University of Science and Technology Key Laboratory of Chemical Additives for China National Light Industry College of Chemistry and Chemical Engineering Shaanxi University of Science and Technology Materials Institute of Atomic and Molecular Science School of Physics & Information Science Shaanxi University of Science and Technology School of Chemistry and Chemical Engineering Shanghai Jiaotong University

Lithium （Li） deposition and nucleation at solid electrolyte interphase （SEI） is the main origin for the capacity decay in Li metal batteries （LMBs）.SEI conversion with enhanced electrochemical and mechanical properties is an effective approach to achieve uniform nucleation of Li+and stabilize the lithium metal ***,complex interfacial reaction mechanisms and interface compatibility issues hinder the development of SEI conversion strategies for stabilizing lithium metal ***,we presented the release of I3-in–NH2-modified metal–organic frameworks for a Li metal surface SEI phase conversion ***–NH2group in MOF pores induced the formation of I3-from I2,which was further spontaneously reacted with inactive Li2O transforming into high-performance LiI and ***,theoretical calculation provided deeply insight into the unique reconstructed interfacial formation and electrochemical mechanism of rich LiI and *** a result,the Li+deposition and nucleation were improved,facilitating the transport kinetics of Li+and inhibiting the growth of lithium *** assembled solid-state Li||LiFePO4full cells exhibited superior long-term stability of 800 cycles and high Coulombic efficiency （>99%）,Li||LiNi0.8Co0.1Mn0.1O2pouch cell also displayed superior practical performance over 200 cycles at 2 C,high loading of 5 mg cm-2and safety *** innovative SEI design strategy promotes the development of high-performance solid-state Li metal batteries.

关键词： Li metal battery MOF Nano-capsule SEI phase conversion Solid electrolyte interphase (SEI) Solid-state electrolytes

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High-efficiency wide-angle anomalous refraction with acoustic metagrating

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Chinese physics B 2025年第1期34卷 368-372页

作者： Kangyao Sun Yuancheng Fan Zhehao Ye Jiahui Li Quanhong Fu Yali Zeng Fuli Zhang MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions School of Physical Science and TechnologyNorthwestern Polytechnical UniversityXi’an 710129China

The emergent metagrating,with its unique and flexible beam shaping capabilities,offers new paths to efficient modulation of acoustic *** this work,an acoustic metagrating is demonstrated for high-efficiency and wide-angle anomalous *** is shown that the normal reflection and transmission can be totally suppressed by properly modulating the amplitude and phase characteristics of the metagrating supercells for high-efficiency anomalous *** anomalous refraction behavior is achieved in the wide range of incident angles from 28°to 78°,and the efficiency of-1st order diffraction is higher than 90%by finely designing the metagrating *** anomalous refraction behaviors are verified experimentally at incidence angle of 28°,45°,and 78°,*** demonstrated metagrating is anticipated to possess efficient wide-angle composite wavefront engineering applications in such fields as communications.

关键词： acoustic metagrating beam steering wide-angle anomalous refraction

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HCl Treatment of Mixed-Phase MoVTeNbO_x Catalysts for Enhanced Performance in Selective Oxidation of Propane

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Precision chemistry 2025年第4期3卷 206-213页

作者： Wei, Zeyue Zhang, Hanzhi Bai, Yunxing Zhang, Xuanyu Huang, Weixin State Key Laboratory of Precision and Intelligent Chemistry iChEM Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes Department of Chemical Physics University of Science and Technology of China Hefei 230026 China

Hydrothermally synthesized mixed-phase MoVTeNbOx catalysts are active for catalyzing the selective oxidation of propane to acrylic acid but suffer from the presence of the amorphous phase and low specific surface area... 详细信息

Hydrothermally synthesized mixed-phase MoVTeNbO_x catalysts are active for catalyzing the selective oxidation of propane to acrylic acid but suffer from the presence of the amorphous phase and low specific surface areas. Herein we report that HCl treatment preferentially dissolves the amorphous phase in hydrothermally synthesized mixed-phase MoVTeNbO_x catalysts and increases the catalytic performance. An optimal HCl treatment significantly increases the C₃H₈ conversion from 38.9% to 58.2% without changing the acrylic acid selectivity in the selective oxidation of propane to acrylic acid at 380 °C. The original and HCl treated catalysts exhibit similar apparent activation energies, while HCl treatment increases the specific surface area, surface acid sites, surface V⁵⁺ density, and C₃H₈ and C₃H₆ irreversible adsorption amounts but decreases the C₃H₈ and C₃H₆ irreversible adsorption heats. The C₃H₈ conversion rate is proportional to the surface V⁵⁺ density and C₃H₈ irreversible adsorption amount, and the TOF is measured as 3.31 ± 0.08 × 10^-5 s^-1 at 340 °C. Thus, HCl treatment enhances the catalytic performance of mixed-phase MoVTeNbO_x catalysts mainly by increasing the active site density rather than by increasing the active site activity. Our results provide an effective approach to prepare highly active mixed-phase MoVTeNbO_x catalysts for the selective oxidation of propane to acrylic acid. © 2025 The Authors. Co-published by University of science and technology of China and American Chemical Society.

关键词： acrylic acid active site microcalorimetry MoVTeNbOx selective oxidation of propane

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A Computer Simulation Study on Deposition Patterns of Cyclic Diblock Copolymer Solution Nanodroplets:Influence of Polymer Length and Concentration

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Chemical Research in Chinese Universities 2025年第1期41卷 21-32页

作者： PEI Hanwen ZHANG Jun SUN Zhaoyan State Key Laboratory of Polymer Physics and Chemistry&Key Laboratory of Polymer Science and Technology Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022P.R.China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei230026P.R.China

Molecular dynamics simulations are conducted to investigate the deposition patterns of cyclic diblock copolymer solution nanodroplets on solid surfaces(walls).The primary focus is how initial polymer concentration,chain length,and solvent-wall interaction affect these *** patterns are categorized into phase diagrams,mainly composed of multihollow,coffee-ring,and multilayer *** also study the deposition of polymer blocks with different adsorption behavior by adjusting the interaction strength between the polymer block and the wall[ε_(A(B)W)],including weakly adsorbable(ε_(A(B)W)=0.6),moderately adsorbable(ε_(A(B)W)=1.0),and strongly adsorbable(εA(B)W=1.2)polymer *** study identifies the key factors influencing the droplet’s deposition structure and elucidates the mechanisms behind pattern *** findings contribute to the design of deposition patterns for cyclic diblock copolymer solution nanodroplets,enhancing applications related to droplet evaporation.

关键词： Cyclic diblock copolymer Nanodroplet Evaporation Deposition pattern Chain length and concentration

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