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Modulating surface oxygen species via facet engineering for efficient conversion of nitrate to ammonia

Journal of Energy Chemistry 2023年第3期78卷 211-221,I0007页

作者： Wenye Zhong Zhiheng Gong Zuyun He Nian Zhang Xiongwu Kang Xianwen Mao Yan Chen School of Environment and Energy State Key Laboratory of Pulp and Paper EngineeringSouth China University of TechnologyGuangzhou 510006GuangdongChina State Key Laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050China Department of Materials Science and Engineering National University of SingaporeSingapore 119077Singapore Institute of Functional Intelligent Materials National University of SingaporeSingapore 119077Singapore Centre for Advanced 2D Materials National University of SingaporeSingapore 119077Singapore

Electrochemical reduction of nitrate,a common pollutant in aquatic environment,to valuable ammonia(NO3-RR) using renewably-sourced electricity has attracted widespread interests,with past efforts mainly focused on designing electrocatalysts with high activity and *** detailed correlation between catalyst properties and NO3-RR kinetics,nevertheless,is still not fully *** this work,we modulate the surface oxygen species of Cu_(2)O via facet engineering,and systematically study the impact of these oxygen species on the NO_(3)^(-)RR *** advanced spectroscopic techniques,densi ty fu n ctional theory calculations and molecular dynamics simulations,we find that while oxygen vacancies on Cu_(2)O(111) surface promote the adsorption of reactants and reaction intermediates,hydroxyl groups effectively inhibit the side reaction of hydrogen evolution and facilitate the hydrogenation process of *** two effects work in concert to render Cu_(2)O(111) facet the highest NO3-RR activity relative to those from other *** study provides critical insights into the synergistic effect of exposed facets and surface oxygen species on heterogeneous catalysis,and offers a generalizable,facet engineeringbased strategy for improving the performance of a variety of electrocatalysts important for renewable energy conversion.

关键词： Facet engineering Oxygen vacancy Hydroxyl group Electrochemical nitrate reduction Ammonia

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Photon number resolvability of multi-pixel superconducting nanowire single photon detectors using a single flux quantum circuit

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Chinese Physics B 2022年第5期31卷 636-640页

作者： Hou-Rong Zhou Kun-Jie Cheng Jie Ren Li-Xing You Li-Liang Ying Xiao-Yan Yang Hao Li Zhen Wang State Key Laboratory of Functional Material for Informatics Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China CAS Center for Excellence in Superconducting Electronics Shanghai 200050China

Superconducting nanowire single-photon detectors(SNSPDs) are typical switching devices capable of detecting single photons with almost 100% detection efficiency. However, they cannot determine the exact number of incident photons during a detection event. Multi-pixel SNSPDs employing multiple read-out channels can provide photon number resolvability(PNR), but they require increased cooling power and costly multi-channel electronic systems. In this work, a single-flux quantum(SFQ) circuit is employed, and PNR based on multi-pixel SNSPDs is successfully demonstrated. A multi-input magnetically coupled DC/SFQ converter(MMD2 Q) circuit with a mutual inductance M is used to combine and record signals from a multi-pixel SNSPD device. The designed circuit is capable of discriminating the amplitude of the combined signals in accuracy of Φ_(0)/M with Φ_(0) being a single magnetic flux quantum. By employing the MMD2 Q circuit,the discrimination of up to 40 photons can be simulated. A 4-parallel-input MMD2 Q circuit is fabricated, and a PNR of3 is successfully demonstrated for an SNSPD array with one channel reserved for the functional verification. The results confirm that an MMD2 Q circuit is an effective tool for implementing PNR with multi-pixel SNSPDs.

关键词： superconducting nanowire single-flux quantum circuit photon number resolution

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Effect of native carbon vacancies on evolution of defects in ZrC_(1-x)under He ion irradiation and annealing

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Journal of materials Science & Technology 2022年第24期119卷 87-97页

作者： Weichao Bao Xin-Gang Wang Ying Lu Ji-Xuan Liu Shikuan Sun Guo-Jun Zhang Fangfang Xu State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsShanghai 200050China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Institute of Functional MaterialsDonghua UniversityShanghai 201620China School of Material Science and Energy Engineering Foshan UniversityFoshan 528000China

The dynamic study of radiation-induced defects with annealing is critical for the material design for nextgeneration nuclear energy *** native vacancy could affect the development of defects,which lacks *** the present work,the as-hot pressed ZrC_(1-x)(x=0,0.15,0.3)ceramics which comprised crystallites of a few microns in size with different amounts of carbon vacancies were irradiated by 540 ke V He^(2+)ions at room temperature with a fluence of 1×10^(17)/cm^(2).The radiation-induced lattice expansion was found to be a common phenomenon in a sequence of ZrC_(0.85)≥ZrC_(1.0)>ZrC_(0.7).Both X-ray and electron diffractions confirmed maintenance of structural integrity without amorphization after *** the irradiated region,only“black-dot”type defects,i.e.,clusters of point defects were observed while no helium-induced cavities,cracks,or extended dislocations were *** as-irradiated ZrC_(1-x)were then annealed at different high *** annealing at 800℃,very tiny helium-induced cavities were found to be generated and the crystal lattice recovered to a great extent,especially for the sub-stoichiometric *** annealed at 1500℃,all the samples almost fully recovered the crystal lattices close to those of as-hot pressed ***,large cavities and extended dislocations were *** increasing amount of native carbon vacancies,the size of cavities increased while the length and density of extended dislocations *** changes of lattice parameters during irradiation and annealing processes have been interpreted by the kinetics of ***,the correlation between native vacancies and damage behavior is discussed.

关键词： Native carbon vacancies Zirconium carbide He ions irradiation Helium bubbles Dislocations

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High-throughput screening of room temperature active Peltier cooling materials in Heusler compounds

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npj Computational materials 2022年第1期8卷 1899-1904页

作者： Huifang Luo Xin Li Yuxiang Wang Yeqing Jin Mingjia Yao Jiong Yang Materials Genome Institute Shanghai UniversityShanghai200444China State Key Laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai200050China Zhejiang Laboratory HangzhouZhejiang311100China

Active Peltier cooling enables Peltier heat transfer in addition to the traditional Fourier thermal conductance,which is useful in some special applications,such as the *** the material wise,however,the study on the active Peltier cooling materials is *** carried out a high-throughput workflow to screen out 5 room-temperature active Peltier cooling materials,GaSbLi_(2),HgPbCa_(2),SnTiRu_(2),GeYbLi_(2),and GeTiFe_(2),from 2958 Heusler *** the five materials are semimetals or very narrow band gap systems with high electrical *** of these materials have relatively large Seebeck coefficients due to the band *** effective thermal conductivityκ_(eff)s,which are the summation of active Peltier thermal conductivity and passive thermal conductivity,are all greater than Cu at the room temperature andΔT=1 *** present work gives a possible way to search active cooling Peltier materials for the applications of precise temperature control.

关键词： conductivity precise Seebeck

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Implementation of an 8-bit bit-slice AES S-box with rapid single flux quantum circuits

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Chinese Physics B 2022年第9期31卷 604-610页

作者： Ruo-Ting Yang Xin-Yi Xue Shu-Cheng Yang Xiao-Ping Gao Jie Ren Wei Yan Zhen Wang State Key Laboratory of Functional Material for Informatics Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050China CAS Center for Excellence in Superconducting Electronics(CENSE) Shanghai 200050China University of Chinese Academy of Sciences Beijing 100049China School of Software and Microelectronics Peking UniversityBeijing 100871China

Rapid single flux quantum(RSFQ)circuits are a kind of superconducting digital circuits,having properties of a natural gate-level pipelining synchronous sequential circuit,which demonstrates high energy efficiency and high throughput *** find that the high-throughput and high-speed performance of RSFQ circuits can take the advantage of a hardware implementation of the encryption algorithm,whereas these are rarely applied to this *** the available encryption algorithms,the advanced encryption standard(AES)algorithm is an advanced encryption standard *** is currently the most widely used symmetric cryptography *** this work,we aim to demonstrate the SubByte operation of an AES-128 algorithm using RSFQ circuits based on the SIMIT Nb0_(3) *** design an AES S-box circuit in the RSFQ logic,and compare its operational frequency,power dissipation,and throughput with those of the CMOS-based circuit post-simulated in the same *** complete RSFQ S-box circuit costs a total of 42237 Josephson junctions with nearly 130 Gbps throughput under the maximum simulated frequency of 16.28 *** analysis shows that the frequency and throughput of the RSFQ-based S-box are about four times higher than those of the CMOS-based ***,we design and fabricate a few typical modules of the *** measurements demonstrate the correct functioning of the modules in both low and high frequencies up to 28.8 GHz.

关键词： RSFQ AES S-box hardware implementation

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Spin Crossover OFF/ON Triggered by Ligand Chemical Doping in an Fe(Ⅲ)Solid Solution

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Chinese Journal of Chemistry 2025年第1期43卷 90-96页

作者： Shuang Peng Yue Gao Zi-Yi Zhang Guang-Yan Xu Wen-Jun Zheng Feng-Lei Yang Jing-Wei Dai Zhao-Yang Li College of Chemistry Nankai University94 Weijin RoadTianjin300071 China School of Materials Science and Engineering Nankai University38 Tongyan RoadTianjin300350 China Jiangsu eKey Laboratory of Green Synthetic Chemistry for Functional Materials School of Chemistry and Material ScienceJiangsu Normal UniversityXuzhouJiangsu221116 China State Key Laboratory of Medicinal Chemical Biology Nankai University94 Weijin RoadTianjin300071 China State Key Laboratory of Elemento-organic Chemistry Nankai University94 Weijin RoadTianjin300071 China

Spin crossover(SCO),characterized by distinct high-spin(HS)and low-spin(LS)states,has potential applications in memory,electronic,and electroluminescent *** OFF/ON switching of SCO is crucial for obtaining bistable magnetic ***,there are few strategies for achieving this ***,based on a ligand chemical doping strategy,we report an Fe(Ⅲ)solid solution that can be prepared using a ligand chemical doping strategy,enabling not only the OFF/ON switching of SCO but also the fine-tuning of the spin transition temperature(T_(c))within a 45 K range near room *** experimental results show that when the polar ligand doping ratio reaches 20%,SCO behavior is triggered,and the crystal phase transforms significantly,becoming loose and ***,T_(c) can be continuously regulated as the ligand-doping ratio *** functional theory(DFT)calculations reveal that solid packing-induced molecular distortion blocks SCO,whereas loosely flexible packing triggers SCO via fluorinated ligand chemical doping.

关键词： Spin crossover OFF/ON switching Room-temperature spin transition Switchable spin transition temperature Ligandchemical doping

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Two-color emissive AIEgens with anti-Kasha property for dual-organelle imaging and phototherapy

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Science China Chemistry 2024年第5期67卷 1740-1752页

作者： Pu Chen Guogang Shan Qingli Nie Yuting Yan Pengfei Zhang Zujin Zhao Hai-Tao Feng Ben Zhong Tang AIE Research Center Shaanxi Key Laboratory of PhytochemistryCollege of Chemistry and Chemical EngineeringBaoji University of Arts and SciencesBaoji 721013China Institute of Functional Material Chemistry and National&Local United Engineering Lab for Power Battery Faculty of ChemistryNortheast Normal UniversityChangchun 130024China College of Chemistry&Materials Science Northwest UniversityXi’an 710127China Guangdong Key Laboratory of Nanomedicine CAS-HK Joint Lab of BiomaterialsCAS Key Laboratory of Biomedical Imaging Science and SystemShenzhen Engineering Laboratory of Nanomedicine and NanoformulationsCAS Key Lab for Health InformaticsShenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China State Key Laboratory of Luminescent Materials and Devices Key Laboratory of Luminescence from Molecular Aggregates of Guangdong ProvinceSouth China University of TechnologyGuangzhou 510640China School of Science and Engineering Shenzhen Institute of Aggregate Science and TechnologyThe Chinese University of Hong KongShenzhen(CUHK-Shenzhen)Shenzhen 518172China

Despite the rapid development of probes for targeting single organelle, the construction of robust dual-organelle targeting probes with multicolor emission was rarely reported. Herein, two dual-emissive aggregation-induced emission luminogens(AIEgens)with donor-π-acceptor structures were designed and synthesized, namely QT-1 and QF-2. Both two AIEgens exhibited excitation wavelength-dependence defying the Kasha's rule, and could stain lipid droplets(LDs) and mitochondria in blue and red fluorescence, respectively. Moreover, thanks to the near-infrared emission and abundant reactive oxygen species(ROS) generation efficiency of QT-1, it was chosen as a photodynamic therapy agent to selectively kill cancer cells from normal cells. Upon light irradiation, an obvious decrease of mitochondrial membrane potential(MMP) and serious change of mitochondrial shape in cells were observed, which corresponded to the efficient inhibition of tumor growth in vivo. This work afforded a promising strategy for the construction of multicolor emission by tuning anti-Kasha behaviors and expanding their application in dualorganelle targeting-based phototheranostics.

关键词： aggregation-induced emission anti-Kasha luminescence fluorescent probe bioimaging photodynamic therapy

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Internal magnetic-field-enhanced photogenerated charge separation in ferromagnetic TiO_(2)surface heterojunctions

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Journal of materials Science & Technology 2023年第29期160卷 240-247页

作者： Guojing Wang Shirong Xiong Yonghui Chen Chunchang Wang Shasha Lv Ke Jia Yunjie Xiang Jianbo Liu Chong Liu Zhengcao Li School of Materials and Energy Lanzhou UniversityLanzhou 730000China State Key Laboratory of New Ceramics and Fine Processing Key Laboratory of Advanced Materials(MOE)School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Laboratory of Dielectric Functional Materials School of Physics and Material ScienceAnhui UniversityHefei 230601China Key Laboratory of Beam Technology Ministry of EducationCollege of Nuclear Science and TechnologyBeijing Normal UniversityBeijing 100875China School of Materials and Energy Southwest UniversityChongqing 404100China

The use of the internal magnetic field of ferromagnets can effectively promote charge separation and transfer(CST)in photoelectrochemical energy ***,photoelectrochemical materials with a ferromagnetic field are scarce,and the internal magnetic field is negligible in nonferromagnetic *** address this issue,we propose a rational method for preparing ferromagnetic TiO_(2)powder using controllable oxygen vacancies in anatase TiO_(2)with co-exposed{001}and{101}***,an ex-cellent saturation magnetisation of 0.0014 emu/g in TiO_(2)is achieved owing to an asymmetric and uneven charge *** with that of nonferromagnetic TiO_(2),the efficiency of photocatalytic hydro-gen generation of ferromagnetic TiO_(2)is improved by 0.64 *** enhancement of photocatalytic hy-drogen generation is due to the different forces exerted on the electrons and holes in the magnetic field,which significantly improve the photogenerated CST efficiency of ferromagnetic TiO_(2).This result high-lights the significant role of the synergistic regulation of the crystal structure and defects in regulating the ferromagnetic characteristics of *** findings of this study provide guidance for leveraging point defects to promote CST for high-efficiency solar-energy conversion systems.

关键词： Photocatalysis TiO_(2){001}-{101}surface heterojunctions Oxygen vacancies Ferromagnetic

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A hybrid nickel/iron-pyromellitic acid electrocatalyst for oxygen evolution reaction

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Nano Research 2024年第4期17卷 2481-2491页

作者： Guoqi Li Lin Li Wenlong Li Fusheng Li Chunze Yuan Nian Zhang Hui Zhang Tsu-Chien Weng School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China Center for Transformative Science ShanghaiTech UniversityShanghai 201210China State Key Lab of Fine Chemicals Institute of Artificial PhotosynthesisDUT-KTH Joint Education and Research Center on Molecular DevicesDalian University of Technology(DUT)Dalian 116024China State Key Laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050China

The migration of protons during the oxygen evolution reaction(OER)is a key factor that affects the performance of OER *** enhance proton transportation,we designed a catalyst based on nickel/iron-pyromellitic acid(NiFe-PMA)prepared by the electrochemical deposition *** catalyst exhibited a low overpotential of 188 mV at a current density of 10 mA·cm^(-2),a Tafel slope of 28.2 mV·dec^(-1),and long-term stability for 30 days with a current of 50 mA·cm^(-2).We characterized the NiFe-PMA catalyst using various techniques,including Fourier transform infrared(FTIR)spectroscopy,Raman spectroscopy,X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),transmission electron microscopy(TEM),scanning electron microscopy(SEM),and inductively coupled plasma-optical emission spectrometry(ICP-OES).Our results showed that NiFe-PMA contains nickel,iron atoms,and both coordinated and uncoordinated carboxylate ***,XPS data confirmed that carboxylate ligands could adjust the outer electronic structure of metal ions,resulting in the high valence state of Ni in *** result of XAS indicated that the nickel atoms present in the catalyst might be easier to maintain a higher chemical *** investigations using kinetic isotope effects(KIEs)and proton inventory revealed that the uncoordinated carboxylic protons played a crucial role in receiving protons during the OER,which promoted the proton transfer of the rate-determining step of the *** novel electrocatalysts provide a new strategy for designing more active and cost-effective catalysts for the OER.

关键词： nickel/iron-pyromellitic acid oxygen evolution reaction kinetic isotope effects

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Engineering electrolyte additives for stable zinc-based aqueous batteries:Insights and prospects

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Journal of Energy Chemistry 2024年第11期98卷 311-326页

作者： Tao Liu Xusheng Dong Bin Tang Ruizheng Zhao Jie Xu Hongpeng Li Shasha Gao Yongzheng Fang Dongliang Chao Zhen Zhou Interdisciplinary Research Center for Sustainable Energy Science and Engineering(IRC4SE2) Engineering Research Center of Advanced Functional Material Manufacturing of Ministry of EducationSchool of Chemical EngineeringZhengzhou UniversityZhengzhou 450001HenanChina Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsState Key Laboratory of Molecular Engineering of Polymers and School of Chemistry and MaterialsFudan UniversityShanghai 200433China College of Mechanical Engineering Yangzhou UniversityYangzhou 225127JiangsuChina

Zn-based aqueous batteries(ZABs) are gaining widespread popularity due to their low cost and high safety profile. However, the application of ZABs faces significant challenges, such as dendrite growth and parasitic reactions of metallic Zn anodes. Therefore, achieving high-energy–density ZABs necessitates addressing the fundamental thermodynamics and kinetics of Zn anodes. Various strategies are available to mitigate these challenges, with electrolyte additive engineering emerging as one of the most efficient and promising approaches. Despite considerable research in this field, a comprehensive understanding of the intrinsic mechanisms behind the high performance of electrolyte additives remains limited. This review aims to provide a detailed introduction to functional electrolyte additives and thoroughly explore their underlying mechanisms. Additionally, it discusses potential directions and perspectives in additive engineering for ZABs, offering insights into future development and guidelines for achieving high-performance ZABs.

关键词： Aqueous batteries Zn anodes Electrolyte additive engineering Interfacial chemistry Electrochemical mechanisms

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