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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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Green Energy & Environment 2024年第7期9卷 1122-1137页

作者： Xiuqing Hao Yuxi Liu Jiguang Deng Lin Jing Jia Wang Wenbo Pei Hongxing Dai Beijing Key laboratory for Green Catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution ControlKey Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaLaboratory of Catalysis Chemistry and NanoscienceDepartment of Chemical EngineeringFaculty of Environment and LifeBeijing University of TechnologyBeijing100124China

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,*** 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.

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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Balancing the Quantum Speed Limit and Instantaneous Energy Cost in Adiabatic Quantum Evolution

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Chinese Physics Letters 2024年第4期41卷 7-12页

作者：徐建文张宇佳郑文蔡浩阳周浩宇李先科廖绪东张钰李邵雄兰栋谭新生于扬 National laboratory of Solid State Microstructures School of PhysicsNanjing UniversityNanjing 210093China Shishan laboratory Suzhou Campus of Nanjing UniversitySuzhou 215163China Hefei National laboratory Hefei 230088China

Adiabatic time-optimal quantum controls are extensively used in quantum technologies to break the constraints imposed by short coherence ***,practically it is crucial to consider the trade-off between the quantum evolution speed and instantaneous energy cost of process because of the constraints in the available control ***,we experimentally show that using a transmon qubit that,even in the presence of vanishing energy gaps,it is possible to reach a highly time-optimal adiabatic quantum driving at low energy cost in the whole evolution *** validates the recently derived general solution of the quantum Zermelo navigation problem,paving the way for energy-efficient quantum control which is usually overlooked in conventional speed-up schemes,including the well-known counter-diabatic *** designing the control Hamiltonian based on the quantum speed limit bound quantified by the changing rate of phase in the interaction picture,we reveal the relationship between the quantum speed limit and instantaneous energy ***,we demonstrate fast and high-fidelity quantum adiabatic processes by employing energy-efficient driving strengths,indicating a promising strategy for expanding the applications of time-optimal quantum controls in superconducting quantum circuits.

关键词： process quantum adiabatic

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Catalysis by subsurface metal atoms in Al(001) through electron transfer

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National Science Review 2024年第4期11卷 12-13页

作者： Bo Sun Ding Ma Beijing National laboratory for Molecular Science New Cornerstone Science Laboratory College of Chemistry and Molecular Engineering Peking University

Heterogeneous catalysis plays a crucial role in the chemical industry, which has evolved from the investigation of chemisorption to an electronic structure[1]. Diverse strategies, such as alloying,doping, and confining, have been applied to enhance the catalytic properties of active sites through electronic modulation. The electron transfer between active sites and substrates profoundly influences catalytic activity [2].

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Recent advances in protein conformation sampling by combining machine learning with molecular simulation

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Chinese Physics B 2024年第3期33卷 80-87页

作者：唐一鸣杨中元姚逸飞周运谈圆王子超潘瞳熊瑞孙俊力韦广红 Department of Physics State Key Laboratory of Surface Physicsand Key Laboratory for Computational Physical Sciences (Ministry of Education)Shanghai 200438China

The rapid advancement and broad application of machine learning(ML)have driven a groundbreaking revolution in computational *** of the most cutting-edge and important applications of ML is its integration with molecular simulations to improve the sampling efficiency of the vast conformational space of large *** review focuses on recent studies that utilize ML-based techniques in the exploration of protein conformational *** first highlight the recent development of ML-aided enhanced sampling methods,including heuristic algorithms and neural networks that are designed to refine the selection of reaction coordinates for the construction of bias potential,or facilitate the exploration of the unsampled region of the energy ***,we review the development of autoencoder based methods that combine molecular simulations and deep learning to expand the search for protein ***,we discuss the cutting-edge methodologies for the one-shot generation of protein conformations with precise Boltzmann ***,this review demonstrates the promising potential of machine learning in revolutionizing our insight into the complex conformational ensembles of proteins.

关键词： machine learning molecular simulation protein conformational space enhanced sampling

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Third-order nonlinear wavelength conversion in chalcogenide glass waveguides towards mid-infrared photonics

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Chinese Physics B 2024年第10期33卷 269-274页

作者： Fengbo Han Jiaxin Gu Lu Huang Hang Wang Yali Huang Xuecheng Zhou Shaoliang Yu Zhengqian Luo Zhipeng Dong Qingyang Du Fujian Key laboratory of Ultrafast Laser Technology and Applications Xiamen UniversityXiamen 361005China Zhejiang laboratory Hangzhou 311100China

The increasing demand in spectroscopy and sensing calls for infrared(mid-IR)light ***,we theoretically investigate nonlinear wavelength conversion of Ge_(28)Sb_(12)Se_(60)chalcogenide glass waveguide in the mid-IR spectral *** waveguide dispersion engineering,we predict generation of over an octave wavelength(2.8μm-5.9μm)tuning range Raman soliton self-frequency shift,over 2.5 octaves wavelength cover range supercontinuum(1.2μm-8.0μm),as well as single soliton Kerr comb generated in suspended Ge_(28)Sb_(12)Se_(60)*** findings evidenced that Ge_(28)Sb_(12)Se_(60)chalcogenide glass waveguides can simultaneously satisfy the generation of Raman soliton self-frequency shift,supercontinuum spectrum,and Kerr frequency comb generation through dispersion engineering towards mid-IR on chip.

关键词： chalcogenide glass Raman soliton self-frequency shift supercontinuum soliton Kerr comb

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Brønsted-acid sites induced photocatalytic cracking of low-polarity polyethylene plastics

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Journal of Energy Chemistry 2024年第9期96卷 509-515页

作者： Qianyou Wen Quan Zhang Zhengzheng Liu Huining Wang Shuya Hao Fan Zhang Lijuan Zhang Qing Han Gengfeng Zheng laboratory of Advanced Materials Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghai 200438China

Polyolefins such as polyethylene(PE)are one of the largest-scale synthetic plastics and play a key role in modern ***,polyethylene is extremely inert to chemical recycling owing to its lack of chemical functionality and low polarity,making it one of the most challenging environmental hazards ***,we developed a phosphorylated CeO_(2)catalyst by an organophosphate precursor and featured efficient photocatalysis of low-density polyethylene(LDPE)without the acid or alkaline *** to pristine CeO_(2),the surface phosphorylation allows to introduce Brønsted acid sites,which facilitate to form carbonium ions on LDPE via *** addition,the suitable band structure of the phosphorylated CeO_(2)catalyst enables efficient photoabsorption and generates reactive oxygen species,leading to the C–C bond cleavage of *** a result,the phosphorylated CeO_(2)catalyst exhibited an outstanding carbon conversion rate of>94%after 48 h of photocatalysis under 50 mW/cm^(2)of simulated sunlight,with a high CO_(2)product selectivity of>99%.Furthermore,the PE microparticles with sizes larger than 10μm released from LDPE plastic wrap were directly and completely degraded by photocatalysis within 12 h,suggesting an attractive and environmentally benign strategy of utilizing solar energy-based photocatalysis for reducing potential hazards of LDPE plastic trashes.

关键词： Photocatalytic cracking Polyethylene Surface phosphorylation Bronsted-acid site Carbon conversion

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Transient long-range distance measurement by a Vernier spectral interferometry

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Photonics Research 2024年第6期12卷 1107-1114页

作者： LIANG XU KUN WANG CHEN LIU WENYING CHEN CHI ZHANG XINLIANG ZHANG Wuhan National laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China Optics Valley laboratory Wuhan 430074China

Rapid and long-range distance measurements are essential in various industrial and scientific applications,and among them,the dual-comb ranging system attracts great attention due to its high ***,the tem-poral asynchronous sampling results in the tradeoff between frame rate and ranging precision,and the non-ambiguity range(NAR)is also limited by the comb cycle,which hinders the further advancement of the dual-comb ranging *** this constraint,we introduce a Vernier spectral interferometry to improve the frame rate and NAR of the ranging ***,leveraging the dispersive time-stretch technology,the dual-comb interferometry becomes spectral ***,the asynchronous time step is unlimited,and the frame rate is improved to 100 ***,dual-wavelength bands are introduced to implement a Vernier spectral interferometry,whose NAR is enlarged from 1.5 m to 1.5 ***,this fast and long-range system also demonstrated high precision,with a 22.91-nm Allan deviation over 10-ms averaging *** a result,the proposed Vernier spectral interferometry ranging system is promising for diverse applications that necessitate rapid and extensive distance measurement.

关键词： interferometry spectral system

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Integrated spatial-temporal random speckle spectrometer with high resolution in the C-band

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Photonics Research 2024年第7期12卷 1556-1563页

作者： SHIBO XU JIAHUI ZHANG JUNWEI CHENG JIANJI DONG Wuhan National laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China Optics Valley laboratory Wuhan 430074China

The increasing demand for diverse portable high-precision spectral analysis applications has driven the rapid development of spectrometer miniaturization. However, the resolutions of existing miniaturized spectrometers mostly remain at the nanometer level, posing a challenge for further enhancement towards achieving picometerlevel precision. Here, we propose an integrated reconstructive spectrometer that utilizes Mach–Zehnder interferometers and a tunable diffraction network. Through random tuning in the time domain and disordered diffraction in the space domain, the random speckle patterns closely related to wavelength information are obtained to construct the transmission matrix. Experimentally, we achieve a high resolution of 100 pm and precisely reconstruct multiple narrowband and broadband spectra. Moreover, the proposed spectrometer features a simple structure, strong portability, and fast sampling speed, which has great potential in the practical application of high-precision portable spectral analysis.

关键词： speckle random resolution

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Production of Functional Materials Derived from Regenerated Silk Fibroin by Utilizing 3D Printing and Biomimetic Enzyme-induced Mineralization

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Chinese Journal of Polymer Science 2024年第3期42卷 299-310,I0005页

作者： Ni Chen Fei-Yu Luo Gong-Wen Yang Jin-Rong Yao Xin Chen Zheng-Zhong Shao State Key laboratory of Molecular Engineering of Polymers Laboratory of Advanced Materials and Department of Macromolecular ScienceFudan UniversityShanghai 200433China

Critical-sized bone defects, commonly encountered in clinical orthopedic surgery, present a significant challenge. One of the promising solutions is to prepare synthetic bone substitute materials with precise structural control, mechanical compatibility, and enhanced osteogenic induction performance, nevertheless the successful preparation of such materials remains difficult. In this study, a two-step technique,integrating an extrusion-based printing process with biomimetic mineralization induced by alkaline phosphatase(ALP), was developed. Initially,a pre-cured hydrogel of regenerated silk fibroin(RSF) with a small quantity of hydroxypropyl cellulose(HPC) and ALP was prepared through heating the mixed aqueous solution. This pre-cured hydrogel demonstrated thixotropic property and could be directly extruded into predetermined structures through a 3D-printer. Subsequently, the 3D-printed RSF-based materials with ALP underwent biomimetic in situ mineralization in calcium glycerophosphate(Ca-GP) mineralizing solution, utilizing the polymer chains of RSF as templates and ALP as a trigger for cleaving phosphate bonds of Ca-GP. The resulting 3D-printed RSF-mineral composites including hydrogel and sponge possessed adjustable compression modulus of megapascal grade and variable hydroxyapatite content, which could be controlled by manipulating the duration of the mineralization ***, these 3D-printed RSF-mineral composites demonstrated non-cytotoxicity towards rat bone marrow mesenchymal stem cells. Therefore, they may hold great potential for applications involving the replacement of tissues characterized by osteoinductivity and intricate structures.

关键词： Silk protein Alkaline phosphatase Extrusion-based printing Biomineralization

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Recent progress on the functionalization of white phosphorus in China

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National Science Review 2024年第6期11卷 308-320页

作者： Xinlei Huangfu Zhongzhen Wang Yu Chen Junnian Wei Wei Liu Wen-Xiong Zhang Beijing National laboratory for Molecular Sciences(BNLMS) State Key Laboratory of Rare-Earth Materials Chemistry and Applications & Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular Engineering Peking University

Direct synthesis of organophosphorus compounds from white phosphorus represents a significant but challenging subject, especially in the context of ongoing efforts to comprehensively improve the phosphorus-derived chemical industry driven by sustainability and safety concerns. China is the world's largest producer of white phosphorus, creating a significant demand for the green transformation of this crucial feedstock. This review provides an overview of advancements in white phosphorus activation by Chinese research teams, focusing on the direct construction of P–C/N/O/S/M bonds from white phosphorus. Additionally, we offer some insights into prospective directions for the activation and transformation of white phosphorus in the future. This review paper aims to attract more researchers to engage in this area, stimulating follow-up exploration and fostering enduring advances.

关键词： white phosphorus organophosphorus compound activation selectivity efficiency

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