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Surface engineering on MnO2 nanorods by La single atoms to accelerate oxygen reduction kinetics

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Rare Metals 2024年第9期43卷 4302-4311页

作者： Zhang-Long He Liu-Qi Wang Min Jiang Jia-Nan Xie Shan Liu Jin-Can Ren Rui Sun Wen-Bin Lv Wei-Bin Guo Yu-Ling Liu Bing Li Qi Liu Hao He School of materials science and engineering Changsha University of Science and Technology School of materials science and engineering NanjingUniversity of Science and Technology School of materials science and engineering Shanghai JiaoTong University Department of Physics City University of Hong Kong

Surface engineering,which modulates the electronic structure and adsorption/desorption properties of electrocatalysts,is one of the key strategies for improving the catalytic ***,we demonstrate a facile solid-phase reaction for surface engineering of MnO2to boost the oxygen reduction *** reaction with surface hydroxy groups,La single atoms with loading amount up to 2.7 wt%are anchored onto *** surface engineering,the oxygen reduction reaction （ORR） kinetics is significantly improved with the half-wave potential from 0.70 to 0.84 V,the number of transferred electrons from 2.5 to 3.9 and the limiting current density from 4.8 to 6.0 mA·*** addition,the catalyst delivers superior discharge performance in both alkaline and neutral metal–air *** functional theory （DFT） calculations reveal that atomic La modulates the surface electronic configuration of MnO2,reduces its d-band center and thus lowers the OOH*and O*reaction energy *** work provides a new route for rational design of highly active electrocatalyst and holds great potential for application in various catalytic reactions.

关键词： Electron injection Metal–air batteries Oxygen reduction reaction Single atoms Surface engineering

“Blocking and rebalance” mechanism-guided design strategies of bimetallic doped 2D a-phosphorus carbide as efficient catalysts for N2 electroreduction

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Journal of Energy Chemistry 2024年第10期97卷 68-78页

作者： Cheng He Jianglong Ma Shen Xi Wenxue Zhang State Key Laboratory for Mechanical Behavior of materials School of Materials Science and Engineering Xi'an Jiaotong University School of materials science and engineering Chang'an University

Compared to single atom catalysts（SACs）,the introduction of dual atom catalysts（DACs） has a significantly positive effect on improving the efficiency in the electrocatalytic nitrogen reduction reaction（NRR） which provides an environmental alternative to the Haber-Bosch ***,the research on the mechanism and strategy of designing bimetallic combinations for better performance is still in its early ***,based on "blocking and rebalance" mechanism,45 combinations of bimetallic pair doped α-phosphorus carbide（TMATMB@PC） are investigated as efficient NRR catalysts through density functional theory and machine learning *** a multi-step screening,the combinations of TiV,TiFe,MnMo,and FeW exhibit highly efficient catalytic performance with significantly lower limiting potentials（-0.17,-0.18,-0.14,and-0.30 V,respectively）.Excitingly,the limiting potential for CrMo and CrW combinations is 0 V,which are considered to be extremely suitable for the NRR *** mechanism of "blocking and rebalance" is revealed by the exploration of charge transfer for phosphorus atoms in electron blocking ***,the descriptor φ is proposed with machine learning,which provides design strategies and accurate prediction for finding efficient *** work not only offers promising catalysts TMATMB@PC for NRR process but also provides design strategies by presenting the descriptor φ.

关键词： 2D α-phosphorus carbide DACs Inherent attributes Machine learning Nitrogen reduction reaction

Dual template-induced construction of three-dimensional porous SiO2/NC/Co-CNTs heterostructure with highly dispersed active sites for efficient oxygen evolution reaction

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Tungsten 2024年第3期6卷 585-595页

作者： Hai-Qi Zhang Xiao-Jun Zeng Qing-Qing Zhang Zu-Liang Zhang Chu-Long Jin Rong-Hai Yu School of materials science and engineering Jingdezhen Ceramic University School of materials science and engineering Beihang University

The development and exploration of efficient and economical electrocatalysts for oxygen evolution reaction（OER） represents the main bottleneck to unlocking a sustainable energy scenario based on elec trocataly tic water *** scale integration of three-dimensional（3D） porous heterostructure with highly dispersed active sites and good structural stability is ***,a dual template route is developed to construct the 3D porous SiO2/nitrogen-doped carbon（NC）/Co-carbon nano tubes（CNTs） hetero ***,the hard template（SiO2nano spheres） contributes to 3D porous structure,increases the specific surface area,and promotes the contact area of the *** the same time,the soft template（basic zinc carbonate） can control the growth of 1D CNTs and facilitate the exposure of the active ***,3D porous SiO2/NC/Co-CNTs hetero structure inherits highly dispersed Co nanoparticles coated by *** conductive channels and abundant N hetero atoms doping are reasonably constructed by a dual template ***,SiO2/NC/Co-CNTs catalyst provides an extraordinary activity for the OER in alkaline media,with a low overpotential of 298 mV at a current density of 10 mA·***,SiO2/NC/Co-CNTs hetero structure enables excellent long-term durability with a 10 mV decay in overpotential after 3000 cyclic voltammetry cycles,and 97% remain in current density over 20 *** is believed that this dual template strategy can provide a new and simple way to construct a highly dispersed active site in electrocatalysts.

关键词： Dual template High dispersion Porous heterostructure Conductive channels Oxygen evolution reaction

Fe-Induced Electronic Transfer and Structural Evolution of Lotus Pod-Like CoNiFePx@P,N-C Heterostructure for Sustainable Oxygen Evolution

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Energy & Environmental materials 2024年第3期7卷 186-193页

作者： Xiaojun Zeng Qingqing Zhang Chulong Jin Hui Huang Yanfeng Gao Advanced Ceramic materials Research Institute School of Materials Science and EngineeringJingdezhen Ceramic University Singapore Institute of Technology School of materials science and engineering Shanghai University

Transition metal phosphides with metallic properties are a promising candidate for electrocatalytic water oxidation,and developing highly active and stable metal phosphide-based oxygen evolution reaction catalysts is still ***,we present a facile ion exchange and phosphating processes to transform intestine-like CoNiPx@P,N-C into lotus pod-like CoNiFePx@P,N-C heterostructure in which numerous P,N-codoped carboncoated CoNiFePxnanoparticles tightly anchors on the 2D carbon ***,the as-prepared CoNiFePx@P,N-C enables a core-shell structure,high specific surface area,and hierarchical pore structure,which present abundant heterointerfaces and fully exposed active ***,the incorporation of Fe can also induce electron transfer in CoNiPx@P,IM-C,thereby promoting the oxygen evolution ***,CoNiFePx@P,IM-C delivers a low overpotential of 278 mV （vs RHE） at a current density of10 mA cm-1and inherits excellent long-term stability with no observable current density decay after 30 h of chronoamperometry *** work not only highlights heteroatom induction to tune the electronic structure but also provides a facile approach for developing advanced and stable oxygen evolution reaction electrocatalysts with abundant heterointerfaces.

关键词： electronic transfer Fe exchange multi-metal phosphides OER electrocatalysts structural evolution

Surface reconstruction of heterostructures in alkaline medium towards enhanced electrocatalytic hydrogen evolution

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Rare Metals 2024年第6期43卷 2636-2647页

作者： Ming-Yang Yang Ji Yuan Xue-Lian Fu Jing-Jing Chen Jing Hu Zhou-Guang Lu Chen Liu Guangdong Research Center for Interfacial engineering of Functional materials Shenzhen Key Laboratory of Polymer Science and TechnologyShenzhen Key Laboratory of Energy Electrocatalytic MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China Shenzhen Key Laboratory of Interfacial science and engineering of materials Department of Materials Science and EngineeringSouthern University of Science and TechnologyShenzhen 518055China

Constructing heterostructures has proved to be a successful strategy to fabricate electrocatalysts with high efficiency for water ***,the structure evolution in alkaline hydrogen evolution reaction lacks investigation and the specific active center remains ***,we take the well-designed Ni_(3)S_(2)@VO_(2) heterostructures as a model to investigate the electrocatalytic activity and the surface reconstruction process of heterostructure catalysts in alkaline *** Ni_(3)S_(2)@VO_(2) heterostructures,with Ni_(3)S_(2) nanorods as the core and VO_(2) nanoflakes as the shell,coupled with the high conductive Ni_(3)S_(2),the hydrophilic VO_(2) and modulated electronic structures at the interfaces,exhibited prominent activity and superior stability at various current ***,the ex-situ characterizations confirmed that the surface reconstruction from Ni_(3)S_(2)@VO_(2) into Ni_(3)S_(2)@amorphous-Ni(OH)_(2) in alkaline media could optimize the water dissociation barrier and exposed large active area,thereby contributing to improved electrocatalytic *** study not only introduces novel high-performance electrocatalysts for hydrogen evolution reaction(HER),but also provides a new avenue for re-examining hetero-structural catalysts in alkaline solutions.

关键词： Heterostructures Ni_(3)S_(2)@VO_(2) Surface reconstruction Water dissociation Alkaline hydrogen evolution

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Boosting cycling stability by regulating surface oxygen vacancies of LNMO by rapid calcination

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Nano Research 2024年第4期17卷 2671-2677页

作者： Haoran Jiang Cuihua Zeng Wei Zhu Jiawei Luo Zhedong Liu Jingchao Zhang Rui Liu Yunhua Xu Yanan Chen Wenbin Hu School of materials science and engineering Tianjin UniversityTianjin 300072China School of materials science and engineering Shandong University of Science and TechnologyQingdao 266590China

Spinel LiNi_(0.5-x)Mn_(1.5+x)O_(4)(LNMO)has attracted intensive interest for lithium-ion battery due to its high voltage and high energy ***,severe capacity fade attributed to unstable surface structure has hampered its *** vacancies(OVs)tend to occur in the surface of the material and lead to surface structure reconstruction,which deteriorates the battery performance during electrochemical ***,we utilize high-temperature-shock(HTS)method to synthesize LNMO materials with fewer surface *** calcination drives lower surface OVs concentration,reducing the content of Mn^(3+)and surface reconstruction layers,which is beneficial to obtain a stable crystal *** LNMO material synthesized by HTS method delivers an initial capacity of 127 mAh·g^(-1) at 0.1 C and capacity retention of 81.6%after 300 cycles at 1 C,and exhibits excellent performance at low temperature.

关键词： ultrafast synthesis oxygen vacancy LiNi_(0.5-x)Mn_(1.5+x)O_(4)(LNMO)cathode high-temperature-shock lithium-ion batteries

Contrasting strategies of optimizing carrier concentration in bulk InSe for enhanced thermoelectric performance

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Rare Metals 2024年第9期43卷 4425-4432页

作者： Hao-Nan Shi Shu-Lin Bai Yu-Ping Wang Li-Zhong Su Qian Cao Cheng Chang Li-Dong Zhao School of materials science and engineering Beihang University School of materials science and engineering Taiyuan University of Science and Technology Huabei Cooling Device Co.Ltd.

Indium selenide (InSe),as a wide-bandgap semiconductor,has received extensive attention in the flexible electronics field in recent years due to its exceptional plasticity and promising thermoelectric ***,the low carrier concentration severely limits its thermoelectric performance *** this work,we conducted contrasting strategies that can be employed to increase the carrier concentration of InSe,including bandgap narrowing and heterovalent ***,the carrier concentration initially increases as a result of the reduced bandgap upon Te alloying and then slightly decreases due to the weak electronegativity of *** Br doping realizes high carrier concentration by pushing the Fermi level into the conduction bands and activating the multiple *** the other hand,both Te and Br obviously suppress the thermal conductivity due to the point defect *** contrast,Br doping realizes a higher thermoelectric performance with a maximum ZT of～0.13 at 773 K benefiting from the better optimization of carrier *** work elucidates the strategies for enhancing carrier concentration at anion sites and demonstrates the high efficiency of halogen doping in ***,the carrier concentration of InSe is promising to be further optimized,and future work should focus on employing approaches such as cation doping or secondphase compositing.

关键词： Bandgap Carrier concentration Heterovalent doping InSe Thermoelectric

On-surface synthesis and characterization of polyynic carbon chains

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National science Review 2024年第3期11卷 192-199页

作者： Wenze Gao Wei Zheng Luye Sun Faming Kang Zheng Zhou Wei Xu Interdisciplinary materials Research Center School of Materials Science and Engineering Tongji University

Carbyne, an elusive sp-hybridized linear carbon allotrope, has fascinated chemists and physicists for decades. Due to its high chemical reactivity and extreme instability, carbyne was much less explored in contrast to the sp2-hybridized carbon allotropes such as graphene. Herein, we report the on-surface synthesis of polyynic carbon chains by demetallization of organometallic polyynes on the Au（111） surface;the longest one observed consists of ～60 alkyne units（120 carbon atoms）. The polyynic structure of carbon chains with alternating triple and single bonds was unambiguously revealed by bond-resolved atomic force microscopy. Moreover, an atomically precise polyyne, C14, was successfully produced via tip-induced dehalogenation and ring-opening of the decachloroanthracene molecule(C14Cl10) on a bilayer NaCl/Au（111） surface at 4.7 K, and a band gap of 5.8 eV was measured by scanning tunnelling spectroscopy,in a good agreement with the theoretical HOMO–LUMO gap（5.48 eV）.

关键词： polyyne scanning probe microscopy carbon allotrope on-surface synthesis organometallic polyyne

Regulating photothermal properties of near-infrared croconaine dyes by supramolecular assembly

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Nano Research 2024年第9期17卷 8560-8570页

作者： Yangge Ren Yue Lu Juanjuan Gao Yi Ding Bo Zhu Xinyu Hou Lin Jia Department of Polymer materials School of Materials Science and EngineeringShanghai UniversityShanghai 200444China Department of Electronic Information materials School of Materials Science and EngineeringShanghai UniversityShanghai 200444China

The photochemical and photophysical properties of near-infrared(NIR)dyes are significantly influenced by their aggregation state and mesoscopic ***,beyond chemical synthesis,the regulation mechanisms for the properties of NIR dyes,particularly with respect to photothermal properties of the aggregates,are not yet fully ***,we investigate the photothermal behaviors of croconaine-based(CroA)NIR dyes containing dipeptide or amino acids *** introduction of hydrogen bonding promotesπ-πstacking of croconaine center,which can efficiently regulate aggregation states and assembly structures in *** laser irradiation,CroA aggregates undergo aggregation-dissociation transition,the in-situ monomer generation process regulates two parameters of photothermal performance:heating rates and plateau photothermal *** study reveals the regulation effect of non-covalent bonding interactions on CroA aggregates,highlighting supramolecular assembly strategy not only facilitates to construct of photothermal nanomaterials with well-defined structures,but also provides an alternative and effective method for regulating photothermal performance of NIR dyes.

关键词： croconaine dye hydrogen bonding photothermal performance supramolecular assembly chirality