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Bimetallic CoNi single atoms supported on three-dimensionally ordered mesoporous chromia:highly active catalysts for n-hexane combustion
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作者 Xiuqing Hao Yuxi Liu +4 位作者 Jiguang Deng Lin Jing Jia Wang Wenbo Pei Hongxing Dai 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第7期1122-1137,共16页
Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile... Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O. 展开更多
关键词 Three-dimensional ordered mesoporous chromium oxide Supported bimetallic single-atom catalyst Cobalt-nickel single atoms n-Hexane combustion Catalytic reaction mechanism
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Potential applications of single-incision laparoscopic totally preperitoneal hernioplasty
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作者 Xiao-Jun Wang Ting Fei +2 位作者 Xiong-Hua Xiang Quan Wang En-Cheng Zhou 《World Journal of Gastrointestinal Surgery》 SCIE 2024年第7期2202-2210,共9页
BACKGROUND The totally preperitoneal(TPP)approach is a new concept that was recently introduced.Although the TPP approach combined with single-incision laparoscopic hernia repair has its own advantages,there is little... BACKGROUND The totally preperitoneal(TPP)approach is a new concept that was recently introduced.Although the TPP approach combined with single-incision laparoscopic hernia repair has its own advantages,there is little evidence reflecting the characteristics and feasibility of either approach.AIM To analyze the potential applications of single-incision laparoscopic TPP(SILTPP)inguinal hernia hernioplasty for the treatment of inguinal hernias.METHODS A total of 152 SIL-TPP surgeries were performed at the First Affiliated Hospital of Ningbo University from February 2019 to November 2022.A single-port,named Iconport,and standard laparoscopic instruments were used during the operation.Demographic data,intraoperative parameters and short-term postoperative outcomes were collected and retrospectively analyzed.RESULTS The demographic data of 152 patients underwent SIL-TPP were shown in Table 1.The average age was 49.5 years(range from 21 to 81 years).The average body mass index was 27.7 kg/m^(2)(range from 17.7 kg/m^(2) to 35.6 kg/m^(2)).SIL-TPP were conducted successfully in 147 patients.Three patients were converted to the SILtransabdominal preperitoneal laparoscopic herniorrhaphy at the initial stage of the study due to a lack of experience.In 2 patients with incisional hernias,an auxiliary operation hole was added during the SIL-TPP procedure,as required for surgery.The mean operative time was 64.5 minutes(range:36.0-110.0 minutes)for unilateral direct and femoral hernias and 81.6 minutes for indirect hernias(range:40.0-150.0 minutes).The mean postoperative hospital stay was 3.4 days.CONCLUSION SIL-TPP is feasible and has advantages for inguinal hernia repair.SIL-TPP has potential benefits for patients with various abdominal wall hernias.Consequently,doctors should be encouraged to actively apply the TPP approach combined with a single incision in their daily work. 展开更多
关键词 Totally preperitoneal hernioplasty Iconport single incision laparoscopic Totally extraperitoneal herniorrhaphy single incision laparoscopic totally preperitoneal hernioplasty
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Single-atom Pt on carbon nanotubes for selective electrocatalysis 被引量:2
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作者 Samuel S.Hardisty Xiaoqian Lin +1 位作者 Anthony R.J.Kucernak David Zitoun 《Carbon Energy》 SCIE EI CAS CSCD 2024年第1期63-71,共9页
Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reactio... Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reaction(HOR).Herein,we describe the synthesis of a Pt single electrocatalyst inside single-walled carbon nanotubes(SWCNTs)via a redox reaction.Characterizations via electron microscopy,X-ray photoelectron microscopy,and X-ray absorption spectroscopy show the single-atom nature of the Pt.The electrochemical behavior of the sample to hydrogen and oxygen was investigated using the advanced floating electrode technique,which minimizes mass transport limitations and gives a thorough insight into the activity of the electrocatalyst.The single-atom samples showed higher HOR activity than state-of-the-art 30%Pt/C while almost no oxygen reduction reaction activity in the proton exchange membrane fuel cell operating range.The selective activity toward HOR arose as the main fingerprint of the catalyst confinement in the SWCNTs. 展开更多
关键词 CONFINEMENT ELECTROCATALYSIS hydrogen PLATINUM single atom catalysts
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Metal-organic framework-based single-atom electro-/ photocatalysts: Synthesis, energy applications, and opportunities 被引量:2
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作者 Munir Ahmad Jiahui Chen +10 位作者 Jianwen Liu Yan Zhang Zhongxin Song Shahzad Afzal Waseem Raza Liaqat Zeb Andleeb Mehmood Arshad Hussain Jiujun Zhang Xian-Zhu Fu Jing-Li Luo 《Carbon Energy》 SCIE EI CAS CSCD 2024年第1期1-43,共43页
Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further de... Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs. 展开更多
关键词 carbon energy generation MOF-derived-supported MOF-supported single atoms
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Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries 被引量:1
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作者 Yugang Qi Qing Liang +9 位作者 Kexin Song Xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Xu Zou Zhongjun Chen Wei Zhang Weitao Zheng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期306-314,I0007,共10页
Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and... Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of interaction.Herein,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery performance.The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic activity.Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion. 展开更多
关键词 ELECTROCATALYTIC Oxygen reduction reaction single atom catalyst Shell coordination optimization
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Advances of Synergistic Electrocatalysis Between Single Atoms and Nanoparticles/Clusters
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作者 Guanyu Luo Min Song +6 位作者 Qian Zhang Lulu An Tao Shen Shuang Wang Hanyu Hu Xiao Huang Deli Wang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第11期377-412,共36页
Combining single atoms with clusters or nanoparticles is an emerging tactic to design efficient electrocatalysts.Both synergy effect and high atomic utilization of active sites in the composite catalysts result in enh... Combining single atoms with clusters or nanoparticles is an emerging tactic to design efficient electrocatalysts.Both synergy effect and high atomic utilization of active sites in the composite catalysts result in enhanced electrocatalytic performance,simultaneously provide a radical analysis of the interrelationship between structure and activity.In this review,the recent advances of single-atomic site catalysts coupled with clusters or nanoparticles are emphasized.Firstly,the synthetic strategies,characterization,dynamics and types of single atoms coupled with clusters/nanoparticles are introduced,and then the key factors controlling the structure of the composite catalysts are discussed.Next,several clean energy catalytic reactions performed over the synergistic composite catalysts are illustrated.Eventually,the encountering challenges and recommendations for the future advancement of synergistic structure in energy-transformation electrocatalysis are outlined. 展开更多
关键词 single atoms NANOPARTICLES CLUSTERS Synergistic composite catalysts Synergistic effect
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Cooperation between single atom catalyst and support to promote nitrogen electroreduction to ammonia:A theoretical insight
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作者 Wanying Guo Siyao Wang +2 位作者 Hongxia Wang Qinghai Cai Jingxiang Zhao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期336-344,共9页
The co-catalysis between single atom catalyst(SAC)and its support has recently emerged as a promising strategy to synergistically boost the catalytic activity of some complex electrochemical reactions,encompassing mul... The co-catalysis between single atom catalyst(SAC)and its support has recently emerged as a promising strategy to synergistically boost the catalytic activity of some complex electrochemical reactions,encompassing multiple intermediates and pathways.Herein,we utilized defective BC_(3)monolayer-supported SACs as a prototype to investigate the cooperative effects of SACs and their support on the catalytic performance of the nitrogen reduction reaction(NRR)for ammonia(NH_(3))production.The results showed that these SACs can be firmly stabilized on these defective BC_(3)supports with high stability against aggregation.Furthermore,co-activation of the inert N_(2)reactant was observed in certain embedded SACs and their neighboring B atoms on certain BC3 sheets due to the noticeable charge transfer and significant N–N bond elongation.Our high-throughput screening revealed that the Mo/DV_(CC)and W/DV_(CC)exhibit superior NRR catalytic performance,characterized by a low limiting potential of−0.33 and−0.43 V,respectively,which can be further increased under acid conditions based on the constant potential method.Moreover,varying NRR catalytic activities can be attributed to the differences in the valence state of active sites.Remarkably,further microkinetic modeling analysis displayed that the turnover frequency of N_(2)–to–NH_(3)conversion on Mo/DV_(CC)is as large as 1.20×10^(−3)s^(−1)site^(−1) at 700 K and 100 bar,thus guaranteeing its ultra-fast reaction rate.Our results not only suggest promising advanced electrocatalysts for NRR but also offer an effective avenue to regulate the electrocatalytic performance via the co-catalytic metal–support interactions. 展开更多
关键词 CO-CATALYSIS single atom catalyst Nitrogen reduction DFT computations
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Thermodynamically induced crystal restructuring to make CsPbCl_(3) single crystal films for weak light detection
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作者 Xiyan Pan Tai An +8 位作者 Jie Sun Hua Dong Zhu Ma Guangxing Liang Yongbo Yuan Yang Li Wuqiang Wu Yong Ding Liming Ding 《Nano Research》 SCIE EI CSCD 2024年第11期9775-9783,共9页
CsPbCl_(3) perovskite is considered a highly promising material for ultraviolet (UV) photodetectors due to its exceptional thermal stability and excellent short-wavelength light response. However, its high lattice ene... CsPbCl_(3) perovskite is considered a highly promising material for ultraviolet (UV) photodetectors due to its exceptional thermal stability and excellent short-wavelength light response. However, its high lattice energy and low polarizability result in extremely low solubility in conventional solvents, making the synthesis of CsPbCl_(3) single crystals a significant challenge. In this study, we propose a novel thermodynamically induced crystal restructuring (TICR) process that can transform microcrystalline films (MCFs) into single crystal films (SCFs) within a short period. This method, for the first time, has successfully achieved the synthesis of centimeter-sized CsPbCl_(3) SCFs and the mechanism has been explored in depth using in-situ techniques. Furthermore, we report the first instance of a CsPbCl_(3) SCF UV photodiode, which exhibits a record-breaking on/off ratio of 3.32 × 10^(7) and a detectivity of up to 1.15 × 10^(14) Jones under 0 V bias. It demonstrates excellent response even under weak light conditions of 10 nW·cm^(−2) and maintains outstanding stability with almost no performance degradation after 15 months. This study provides a novel approach for the synthesis of perovskite single crystals and holds significant potential for advancing the development of high-performance optoelectronic devices. 展开更多
关键词 CsPbCl3 single crystal film crystal restructuring PHOTODIODE ultraviolet detector
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Preparation of single atom catalysts for high sensitive gas sensing
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作者 Xinxin He Ping Guo +7 位作者 Xuyang An Yuyang Li Jiatai Chen Xingyu Zhang Lifeng Wang Mingjin Dai Chaoliang Tan Jia Zhang 《International Journal of Extreme Manufacturing》 SCIE EI CAS CSCD 2024年第3期216-248,共33页
Single atom catalysts(SACs)have garnered significant attention in the field of catalysis over the past decade due to their exceptional atom utilization efficiency and distinct physical and chemical properties.For the ... Single atom catalysts(SACs)have garnered significant attention in the field of catalysis over the past decade due to their exceptional atom utilization efficiency and distinct physical and chemical properties.For the semiconductor-based electrical gas sensor,the core is the catalysis process of target gas molecules on the sensitive materials.In this context,the SACs offer great potential for highly sensitive and selective gas sensing,however,only some of the bubbles come to the surface.To facilitate practical applications,we present a comprehensive review of the preparation strategies for SACs,with a focus on overcoming the challenges of aggregation and low loading.Extensive research efforts have been devoted to investigating the gas sensing mechanism,exploring sensitive materials,optimizing device structures,and refining signal post-processing techniques.Finally,the challenges and future perspectives on the SACs based gas sensing are presented. 展开更多
关键词 single atom catalysts PREPARATION sensing mechanism gas sensing
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Enhancing thermodynamic stability of single-crystal Ni-rich cathode material via a synergistic dual-substitution strategy
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作者 Jixue Shen Hui Li +6 位作者 Haoyu Qi Zhan Lin Zeheng Li Chuanbo Zheng Weitong Du Hao Chen Shanqing Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期428-436,I0010,共10页
Nickel(Ni)-rich cathode materials have become promising candidates for the next-generation electrical vehicles due to their high specific capacity.However,the poor thermodynamic stability(including cyclic performance ... Nickel(Ni)-rich cathode materials have become promising candidates for the next-generation electrical vehicles due to their high specific capacity.However,the poor thermodynamic stability(including cyclic performance and safety performance or thermal stability)will restrain their wide commercial application.Herein,a single-crystal Ni-rich Li Ni_(0.83)Co_(0.12)Mn_(0.05)O_(2) cathode material is synthesized and modified by a dual-substitution strategy in which the high-valence doping element improves the structural stability by forming strong metal–oxygen binding forces,while the low-valence doping element eliminates high Li^(+)/Ni^(2+)mixing.As a result,this synergistic dual substitution can effectively suppress H2-H3 phase transition and generation of microcracks,thereby ultimately improving the thermodynamic stability of Ni-rich cathode material.Notably,the dual-doped Ni-rich cathode delivers an extremely high capacity retention of 81%after 250 cycles(vs.Li/Li+)in coin-type half cells and 87%after 1000 cycles(vs.graphite/Li^(+))in pouch-type full cells at a high temperature of 55℃.More impressively,the dual-doped sample exhibits excellent thermal stability,which demonstrates a higher thermal runaway temperature and a lower calorific value.The synergetic effects of this dual-substitution strategy pave a new pathway for addressing the critical challenges of Ni-rich cathode at high temperatures,which will significantly advance the high-energy-density and high-safety cathodes to the subsequent commercialization. 展开更多
关键词 Ni-rich cathode single crystalline Dual-substitution strategy High-temperature cathode Li-ion batteries
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Electrocatalytic organic transformation reactions in green chemistry: Exploring nanocrystals and single atom catalysts
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作者 Ziwei Deng Yuexin Guo +3 位作者 Zhiyi Sun Jie Lin Huazhang Zhai Wenxing Chen 《Nano Research》 SCIE EI CSCD 2024年第11期9326-9344,共19页
Organic synthesis chemistry plays a crucial role in supporting social sustainable development and finds widespread applications across various fields. Electrocatalysis, with its benefits of high efficiency, mild react... Organic synthesis chemistry plays a crucial role in supporting social sustainable development and finds widespread applications across various fields. Electrocatalysis, with its benefits of high efficiency, mild reaction conditions, controllability, and environmental friendliness, stands out as one of the most effective strategies for driving the transformation of organic substrates. In recent years, nanocrystals (NCs) and single atom catalysts (SACs) have garnered significant attention in the realm of electrocatalytic organic transformation. This article presents a comprehensive overview of the applications of NCs and SACs in electrocatalytic organic transformation. It delves into advanced catalysts for electrocatalysis of representative substrates, covering both anodic oxidation and cathodic reduction aspects, and addresses their synthesis, characterization, catalytic mechanism, and performance. The ultimate goal of this review is to serve as a valuable reference and a source of inspiration for further exploration into the development of more effective catalysts for electrocatalytic organic transformation. 展开更多
关键词 single atom catalysts NANOCRYSTALS electrocatalysis organic transformation
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Highly Sensitive Ammonia Gas Sensors at Room Temperature Based on the Catalytic Mechanism of N,C Coordinated Ni Single-Atom Active Center
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作者 Wenjing Quan Jia Shi +10 位作者 Min Zeng Wen Lv Xiyu Chen Chao Fan Yongwei Zhang Zhou Liu Xiaolu Huang Jianhua Yang Nantao Hu Tao Wang Zhi Yang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第12期515-531,共17页
Significant challenges are posed by the limitations of gas sensing mechanisms for trace-level detection of ammonia(NH3).In this study,we propose to exploit single-atom catalytic activation and targeted adsorption prop... Significant challenges are posed by the limitations of gas sensing mechanisms for trace-level detection of ammonia(NH3).In this study,we propose to exploit single-atom catalytic activation and targeted adsorption properties to achieve highly sensitive and selective NH3 gas detection.Specifically,Ni singleatom active sites based on N,C coordination(Ni-N-C)were interfacially confined on the surface of two-dimensional(2D)MXene nanosheets(Ni-N-C/Ti_(3)C_(2)Tx),and a fully flexible gas sensor(MNPE-Ni-N-C/Ti_(3)C_(2)Tx)was integrated.The sensor demonstrates a remarkable response value to 5 ppm NH3(27.3%),excellent selectivity for NH3,and a low theoretical detection limit of 12.1 ppb.Simulation analysis by density functional calculation reveals that the Ni single-atom center with N,C coordination exhibits specific targeted adsorption properties for NH3.Additionally,its catalytic activation effect effectively reduces the Gibbs free energy of the sensing elemental reaction,while its electronic structure promotes the spill-over effect of reactive oxygen species at the gas-solid interface.The sensor has a dual-channel sensing mechanism of both chemical and electronic sensitization,which facilitates efficient electron transfer to the 2D MXene conductive network,resulting in the formation of the NH3 gas molecule sensing signal.Furthermore,the passivation of MXene edge defects by a conjugated hydrogen bond network enhances the long-term stability of MXene-based electrodes under high humidity conditions.This work achieves highly sensitive room-temperature NH3 gas detection based on the catalytic mechanism of Ni single-atom active center with N,C coordination,which provides a novel gas sensing mechanism for room-temperature trace gas detection research. 展开更多
关键词 Gas sensor single atom Catalytic activation Targeted adsorption End-sealing passivation
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Purification of copper foils driven by single crystallization
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作者 寇金宗 赵孟泽 +10 位作者 李兴光 何梦林 杨方友 刘科海 成庆秋 任云龙 刘灿 付莹 吴慕鸿 刘开辉 王恩哥 《Chinese Physics B》 SCIE EI CAS CSCD 2024年第2期506-511,共6页
High-purity copper(Cu) with excellent thermal and electrical conductivity, is crucial in modern technological applications, including heat exchangers, integrated circuits, and superconducting magnets. The current puri... High-purity copper(Cu) with excellent thermal and electrical conductivity, is crucial in modern technological applications, including heat exchangers, integrated circuits, and superconducting magnets. The current purification process is mainly based on the zone/electrolytic refining or anion exchange, however, which excessively relies on specific integrated equipment with ultra-high vacuum or chemical solution environment, and is also bothered by external contaminants and energy consumption. Here we report a simple approach to purify the Cu foils from 99.9%(3N) to 99.99%(4N) by a temperature-gradient thermal annealing technique, accompanied by the kinetic evolution of single crystallization of Cu.The success of purification mainly relies on(i) the segregation of elements with low effective distribution coefficient driven by grain-boundary movements and(ii) the high-temperature evaporation of elements with high saturated vapor pressure.The purified Cu foils display higher flexibility(elongation of 70%) and electrical conductivity(104% IACS) than that of the original commercial rolled Cu foils(elongation of 10%, electrical conductivity of ~ 100% IACS). Our results provide an effective strategy to optimize the as-produced metal medium, and therefore will facilitate the potential applications of Cu foils in precision electronic products and high-frequency printed circuit boards. 展开更多
关键词 PURIFICATION copper foil thermal annealing technique single crystallization
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Cryptanalysis of efficient semi-quantum secret sharing protocol using single particles
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作者 高甘 《Chinese Physics B》 SCIE EI CAS CSCD 2024年第4期254-257,共4页
In paper[Chin.Phys.B 32070308(2023)],Xing et al.proposed a semi-quantum secret sharing protocol by using single particles.We study the security of the proposed protocol and find that it is not secure,that is,the three... In paper[Chin.Phys.B 32070308(2023)],Xing et al.proposed a semi-quantum secret sharing protocol by using single particles.We study the security of the proposed protocol and find that it is not secure,that is,the three dishonest agents,Bob,Charlie and Emily can collude to obtain Alice's secret without the help of David. 展开更多
关键词 security loophole rearranging orders semi-quantum secret sharing single particles
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Single crystal growth and transport properties of narrow-bandgap semiconductor RhP_(2)
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作者 吴德胜 郑萍 雒建林 《Chinese Physics B》 SCIE EI CAS CSCD 2024年第8期545-549,共5页
We report the growth of high-quality single crystals of RhP_(2),and systematically study its structure and physical properties by transport,magnetism,and heat capacity measurements.Single-crystal x-ray diffraction rev... We report the growth of high-quality single crystals of RhP_(2),and systematically study its structure and physical properties by transport,magnetism,and heat capacity measurements.Single-crystal x-ray diffraction reveals that RhP_(2) adopts a monoclinic structure with the cell parameters a=5.7347(10)A,b=5.7804(11)A,and c=5.8222(11)A,space group P2_(1)/c(No.14).The electrical resistivityρ(T)measurements indicate that RhP_(2) exhibits narrow-bandgap behavior with the activation energies of 223.1 meV and 27.4 meV for two distinct regions,respectively.The temperaturedependent Hall effect measurements show electron domain transport behavior with a low charge carrier concentration.We find that RhP_(2) has a high mobilityμ_(e)~210 cm^(2)·V^(-1)·s^(-1)with carrier concentrations n_(e)~3.3×10^(18)cm^(3) at 300 K with a narrow-bandgap feature.The high mobilityμ_(e) reaches the maximum of approximately 340 cm^(2)·V^(-1)·s^(-1)with carrier concentrations n_^(e)~2×10^(18)cm^(-3)at 100 K.No magnetic phase transitions are observed from the susceptibilityχ(T)and specific heat C_(p)(T)measurements of RhP_(2).Our results not only provide effective potential as a material platform for studying exotic physical properties and electron band structures but also motivate further exploration of their potential photovoltaic and optoelectronic applications. 展开更多
关键词 single crystal growth narrow band system electrical transport high mobilities
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Achieving Negatively Charged Pt Single Atoms on Amorphous Ni(OH)_(2)Nanosheets with Promoted Hydrogen Absorption in Hydrogen Evolution
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作者 Yue Liu Gui Liu +6 位作者 Xiangyu Chen Chuang Xue Mingke Sun Yifei Liu Jianxin Kang Xiujuan Sun Lin Guo 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第10期213-224,共12页
Single-atom(SA)catalysts with nearly 100%atom utilization have been widely employed in electrolysis for decades,due to the outperforming catalytic activity and selectivity.However,most of the reported SA catalysts are... Single-atom(SA)catalysts with nearly 100%atom utilization have been widely employed in electrolysis for decades,due to the outperforming catalytic activity and selectivity.However,most of the reported SA catalysts are fixed through the strong bonding between the dispersed single metallic atoms with nonmetallic atoms of the substrates,which greatly limits the controllable regulation of electrocatalytic activity of SA catalysts.In this work,Pt-Ni bonded Pt SA catalyst with adjustable electronic states was successfully constructed through a controllable electrochemical reduction on the coordination unsaturated amorphous Ni(OH)_(2)nanosheet arrays.Based on the X-ray absorption fine structure analysis and first-principles calculations,Pt SA was bonded with Ni sites of amorphous Ni(OH)_(2),rather than conventional O sites,resulting in negatively charged Pt^(δ-).In situ Raman spectroscopy revealed that the changed configuration and electronic states greatly enhanced absorbability for activated hydrogen atoms,which were the essential intermediate for alkaline hydrogen evolution reaction.The hydrogen spillover process was revealed from amorphous Ni(OH)_(2)that effectively cleave the H-O-H bond of H_(2)O and produce H atom to the Pt SA sites,leading to a low overpotential of 48 mV in alkaline electrolyte at-1000 mA cm^(-2)mg^(-1)_(Pt),evidently better than commercial Pt/C catalysts.This work provided new strategy for the control-lable modulation of the local structure of SA catalysts and the systematic regulation of the electronic states. 展开更多
关键词 Hydrogen evolution reaction AMORPHOUS Pt single atoms Hydrogen spillover
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Application of metal-based catalysts for Fenton reaction: from homogeneous to heterogeneous, from nanocrystals to single atom
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作者 Shangkun Pei Sheng Wang +2 位作者 Yuxin Lu Xiang Li Bo Wang 《Nano Research》 SCIE EI CSCD 2024年第11期9446-9471,共26页
Nowadays, increasing emissions of hazardous chemicals cause serious environmental pollution. The advanced oxidation processes (AOPs), which produce numbers of reactive oxygen species (ROS), are one of the most widely ... Nowadays, increasing emissions of hazardous chemicals cause serious environmental pollution. The advanced oxidation processes (AOPs), which produce numbers of reactive oxygen species (ROS), are one of the most widely used technologies for degrading refractory pollutants in aqueous phase. Among these, Fenton reaction including both homogeneous and heterogeneous processes, has received increasing attention for water treatment. In this review, various nanomaterials with different size such as nanocrystals, nanoparticles (e.g., iron-based minerals, bimetallic oxides, zero-valent iron, quantum dots) and metal-based single atom catalysts (SACs) applied in homogeneous and heterogeneous Fenton reactions, as well as the corresponding catalytic mechanisms will be systematically summarized. Several factors including the morphology, chemical composition, geometric/electronic structures influence the catalytical behavior simultaneously. Here, the recent research advancement including the advantages and further challenges in homogeneous and heterogeneous Fenton system will be introduced in detail. Furthermore, developments for different nanomaterials, from nanocrystals, nanoparticles (minerals, bimetallic oxides represented by Fe-based catalysts, and nanosized zero valent iron materials) to SACs will be discussed. Some representative catalysts for Fenton reaction and their applications will be presented. In addition, commonly-used supports (e.g., graphene oxide, g-C3N4, and carbon nanotubes) and metal-organic frameworks (MOFs)/derivatives and metal-support interaction for improving Fenton-like performance will be introduced. Finally, different types of catalysts for Fenton reaction are compared and their practical application and operational costs are summarized. 展开更多
关键词 NANOCRYSTALS water purification NANOMATERIALS single atom catalysts(SACs) heterogeneous reaction
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Oxidation behavior of 4774DD1 Ni-based single-crystal superalloy at 980℃ in air
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作者 Yu Fang Ya-zhou Li +7 位作者 Qiang Yang Qun-gong He Xiu-fang Gong Qian Duan Hai-yang Song Fu Wang Qiong-yuan Zhang Hong Zeng 《China Foundry》 SCIE EI CAS CSCD 2024年第2期116-124,共9页
The oxidation behavior of a novel Ni-based single-crystal 4774DD1 superalloy for industrial gas turbine applications was investigated by the isothermal oxidation at 980℃ and discontinuous oxidation weight gain method... The oxidation behavior of a novel Ni-based single-crystal 4774DD1 superalloy for industrial gas turbine applications was investigated by the isothermal oxidation at 980℃ and discontinuous oxidation weight gain methods.The phase constitution and morphology of surface oxides and the characteristics of the crosssection oxide film were analyzed by XRD,SEM and EDS.Results show that the oxidation kinetics of the 4774DD1 superalloy follows the cubic law,indicating its weak oxidation resistance at this temperature.As the oxidation time increases,the composition of the oxide film evolves as following:One layer consisting of a bottom Al_(2)O_(3)sublayer and an upper(Al_(2)O_(3)+NiO)mixture sublayer after oxidized for 25 h.Then,two layers composed of an outermost small NiO discontinuous grain layer and an internal layer for 75 h.This internal layer is consisted of the bottom Al_(2)O_(3)sublayer,an intermediate narrow CrTaO_(4)sublayer,and an upper(Al_(2)O_(3)+NiO)mixture sublayer.Also two layers comprising an outermost relative continuous NiO layer with large grain size and an internal layer as the oxidation time increases to 125 h.This internal layer is composed of the upper(Al_(2)O_(3)+NiO)mixture sublayer,an intermediate continuous(CrTaO_(4)+NiWO_(4))mixture sublayer,and a bottom Al_(2)O_(3)sublayer.Finally,three layers consisting of an outermost(NiAl2O_(4)+NiCr2O_(4))mixture layer,an intermediate(CrTaO_(4)+NiWO_(4))mixture layer,and a bottom Al_(2)O_(3)layer for 200 h. 展开更多
关键词 nickel-base single crystal superalloy oxidation kinetics oxide film MICROSTRUCTURE mechanism
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Structure design and electrochemical properties of carbon-based single atom catalysts in energy catalysis:A review
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作者 Shuqi Li Xincheng Lu +8 位作者 Shuling Liu Jingjing Zhou Yanyan Liu Huanhuan Zhang Ruofan Shen Kang Sun Jianchun Jiang Yongfeng Wang Baojun Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第11期196-236,共41页
Single atom catalysts(SACs) possessing regulated electronic structure, high atom utilization, and superior catalytic efficiency have been studied in almost all fields in recent years. Carbon-based supporting SACs are ... Single atom catalysts(SACs) possessing regulated electronic structure, high atom utilization, and superior catalytic efficiency have been studied in almost all fields in recent years. Carbon-based supporting SACs are becoming popular materials because of their low cost, high electron conductivity, and controllable surface property. At the stage of catalysts preparation, the rational design of active sites is necessary for the substantial improvement of activity of catalysts. To date, the reported design strategies are mainly about synthesis mechanism and synthetic method. The level of understanding of design strategies of carbon-based single atom catalysts is requiring deep to be paved. The design strategies about manufacturing defects and coordination modulation of catalysts are presented. The design strategies are easy to carry out in the process of drawing up preparation routes. The components of carbon-based SACs can be divided into two parts: active site and carbon skeleton. In this review, the manufacture of defects and coordination modulation of two parts are introduced, respectively. The structure features and design strategies from the active sites and carbon skeletons to the overall catalysts are deeply discussed.Then, the structural design of different nano-carbon SACs is introduced systematically. The characterization of active site and carbon skeleton and the detailed mechanism of reaction process are summarized and analyzed. Next, the applications in the field of electrocatalysis for oxygen conversion and hydrogen conversion are illustrated. The relationships between the superior performance and the structure of active sites or carbon skeletons are discussed. Finally, the conclusion of this review and prospects on the abundant space for further promotion in broader fields are depicted. This review highlights the design and preparation thoughts from the parts to the whole. The detailed and systematic discussion will provide useful guidance for design of SACs for readers. 展开更多
关键词 Carbon materials Coordination chemistry Defective structure Energy catalysis single atom catalysts
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Comparative analysis of single-crater parameters in ultrasonic-assisted and unassisted micro-EDM of Ti6Al4V using discharge plasma imaging
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作者 Sohaib Raza Chandrakant Nirala 《Nanotechnology and Precision Engineering》 EI CAS CSCD 2024年第2期11-24,共14页
Ultrasonic-assisted micro-electro-discharge machining(EDM)has the potential to enhance processing responses such as material removal rate(MRR)and surface finish.To understand the reasons for this enhancement,the physi... Ultrasonic-assisted micro-electro-discharge machining(EDM)has the potential to enhance processing responses such as material removal rate(MRR)and surface finish.To understand the reasons for this enhancement,the physical mechanisms responsible for the individual discharges and the craters that they form need to be explored.This work examines features of craters formed by single discharges at various parameter values in both conventional and ultrasonic-assistedEDM of Ti6Al4V.High-speed imaging of the plasma channel is performed,and data on the individual discharges are captured in real-time.A 2D axisymmetric model using finite element software is established to model crater formation.On the basis of simulation and experimental results,a comparative study is then carried out to examine the effects of ultrasonic vibrational assistance on crater geometry.For every set ofEDM parameters,the crater diameter and depth from a single discharge are found to be higher in ultrasonic-assistedEDM than in conventionalEDM.The improved crater geometry and the reduced bulge formation at the crater edges are attributed to the increased melt pool velocity and temperature predicted by the model. 展开更多
关键词 Ultrasonic vibration Discharge crater Plasma diameter single discharge
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