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Tailoring the surface and interface structures of photocatalysts to enhance hydrogen production

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Science China Chemistry 2024年第4期67卷 1161-1174页

作者： Tao Zhang Pengfei Wang Shuai Yue Fei Li Zhiyong Zhao Sihui Zhan moe Key Laboratory of Pollution Processes and Environmental Criteria/Tianjin Key Laboratory of Environmental Remediation and Pollution control College of Environmental Science and EngineeringNankai UniversityTianjin 300350China

Photocatalytic water splitting using semiconductor photocatalysts is a promising approach for the production of carbon-neutral,sustainable and clean hydrogen fuel.However,the separation and transport of photoinduced carriers are generally considered to be rate-limiting steps,and their low efficiency remains a major challenge.Therefore,much effort has been devoted to developing new strategies in surface/interface engineering of photocatalysts to improve the dynamics of charge separation/transport.This feature article briefly summarizes recent advances in photocatalyst surface/interface engineering by our research group,which have been achieved through the design of various novel photocatalysts,including interfacial modulation,heterostructure construction,heteroatom doping,single atom and diatom sites.The article is divided into three parts:first,we briefly introduce the three key processes involved in solar water splitting and reveal relationships between the properties of nanostructural photocatalysts and the fundamentals of water splitting;second,we detail methods and strategies for surface and interfacial structures to improve the efficiency of the fundamental processes,especially charge separation;finally,we explore prospects for photocatalytic water splitting applications.This article provides a valuable resource and strategies for researchers currently working in the field of photocatalytic water splitting.

关键词： photocatalytic water splitting surface/interface structures dual-functional photocatalysis

Selection of Suitable Area and Analysis of Adaptability Difference of Prunus humilis

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Asian Agricultural Research 2024年第3期16卷 41-45页

作者： Ze YAO Shengxiu JIANG Zizhu YAN Qi WANG Dawei WANG Gansu Desert control Research Institute Lanzhou 730700China Gansu Psammophytes engineering Technology Research center Lanzhou 730700China State Key Laboratory of desertification and Aeolian sand Disaster Combating Lanzhou 730700China

This paper delves into and assesses the differences in biological traits and fruit nutritional composition of 3 varieties of Prunus humilis introduced from 2 different regions.Results showed that(i)the contents of protein,total sugar,and calcium of No.5 variety were higher those of the other 2 varieties,which was recognized as the most suitable variety for fresh fruit;(ii)the comparison of leaf areas index and fruit shape index of 3 varieties shows that the fruit shape index and individual fruit weight of the introduced varieties were higher than those of the control,the diameter of individual fruit of the introduced varieties higher than that of the control indicated that they had a higher fruit hardness,more dry matter accumulation and better fruit quality,and that the introduction region was more suitable for scale-up of P.humilis;(iii)there was a positive correlation with the number of fruiting branches and there was a significant negative correlation with individual fruit weight,while the leaf area had a significant negative correlation with the number of fruiting branches.The introduced varieties can develop normally in the 2 testing areas,notably,No.5 variety performed better than No.4 and No.6.Improving management is the prerequisite for maintaining proper number of fruiting branches and high yield.

关键词： Prunus humilis Biological traits Nutritional components Introduction and cultivation

Key progresses of moe key laboratory of macromolecular synthesis and functionalization in 2022

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Chinese Chemical Letters 2024年第3期35卷 114-126页

作者： Xumeng Deng Kaihao Chen Kai Pang Xiaoting Liu Minsong Gao Jie Ren Guanwen Yang Guangpeng Wu Chengjian Zhang Xufeng Ni Peng Zhang Jian Ji Jianzhao Liu Zhengwei Mao Ziliang Wu Zhen Xu Haoke Zhang Hanying Li moe Key Laboratory of Macromolecular Synthesis and Functionalization International Research Center for X PolymersDepartment of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China

In 2022,The moe Key Laboratory of Macromolecular Synthesis and Functionalization in Zhejiang University had achieved several important results.First,a series of well-defined dinuclear organoboron catalysts were developed to precisely control the enchainment of ether and carbonate segments during the copolymerization of CO_(2)and epoxides.Second,polyester had been synthesized through cationic copolymerization of cyclic anhydride.Third,ring-opening polymerization of carbon dioxide based valerolactone had been achieved,revealing the prospect of 3-ethylidene-6-vinyltetrahydro-2H-pyran-2-one(EVL)in utilizing CO_(2)and synthesizing functional polymers.Fourth,machine learning methods have been applied to biomaterial research,enabling high-throughput screening of functional biomaterial surfaces for implantable devices,and searching for potent antimicrobial peptides in whole combinatorial peptide libraries.Fifth,methods of characterization of biomacromolecule RNA transcription and manipulation of nucleoside modification were developed.Sixth,artificial enzymes-armed Bifidobacterium Longum probiotics were established to tune down gut inflammation.Seventh,three-dimensional(3D)printing technologies were used to engineer tough supramolecular hydrogels.Eighth,hydroplastic foaming graphene frameworks for acoustic and conductive polymer composites were provided for application.Ninth,aggregate photophysics about the nature of through-space interactions(TSIs)and manipulating their strength in small molecules with non-conjugated structure had been elucidated.Tenth,the forming mechanism of a newfound nested texture in poly(L-lactic acid)(PLLA)spherulitic films had been revealed.Finally,the isotropically dyeing mechanism of KDP single crystals grown from hydrogels have been explored.The related works are reviewed in this paper.

关键词： Polymer Catalyst Biomaterial research mRNA Hydrogel Graphene Crystal

Kinetically and thermodynamically expediting elementary steps via high-valence Cr-incorporated of nickel selenide for water electrolysis

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Nano Research 2024年第3期17卷 1199-1208页

作者： Huafeng Fan Dongxu Jiao Jinchang Fan Dewen Wang Bilal Zaman Wei Zhang Lei Zhang Weitao Zheng Xiaoqiang Cui State Key Laboratory of Automotive Simulation and control School of Materials Science and EngineeringKey Laboratory of Automobile Materials of MOEJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy CenterJilin UniversityChangchun 130012China College of Chemistry Jilin UniversityChangchun 130012China

Designing high-performance electrocatalysts toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is essential to reduce the activation barrier and optimize free adsorption energy of reactive intermediates.Herein,we report that incorporating high-valence Cr into NiSe_(2)(Cr_(x)Ni_(1-x)Se_(2))kinetically and thermodynamically expedites elementary steps of both HER and OER.The as-prepared Cr_(0.05)Ni_(0.95)Se_(2) catalyst displays excellent HER and OER activities,with low overpotentials of 89 and 272 mV at the current density of 10 mA·cm^(-2)(j10),respectively,and remains stable during operation for 30 h.A low cell voltage of only 1.59 V is required to drive j10 in alkaline media.In situ Raman spectroscopy reveals that Cr incorporation facilitates the formation of NiOOH active species during the OER process.Meanwhile,theoretical explorations demonstrate that high-valence Cr incorporation efficiently accelerates water dissociation kinetics and improves H*adsorption during HER process,lowering the activation barrier of OER and optimizing the adsorption energy of oxygen-based intermediate,thus kinetically and thermodynamically enhancing the intrinsic performance of NiSe_(2) for over water splitting.This strategy provides a new horizon to design transition metal based electrocatalysts in the clean energy field.

关键词： nickel selenide electrocatalytic water splitting high-valence Cr density functional theory(DFT)calculation

A polarization sensitive interferometer:Delta interferometer

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Chinese Physics B 2024年第3期33卷 369-377页

作者：卫超奇刘建彬董翼飞孙雨农周宇郑淮斌刘严严闫秀生李福利徐卓 Key Laboratory of Multifunctional Materials and Structures Ministry of Education & International Center for Dielectric ResearchSchool of Electronic Science and EngineeringXi'an Jiaotong UniversityXi'an 710049China moe Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter Department of Applied PhysicsXi'an Jiaotong UniversityXi'an 710049China Science and Technology on Electro-Optical Information Security control Laboratory Tianjin 300308China

A new type of polarization sensitive interferometer is proposed,named the Delta interferometer,inspired by its geometry resembling the Greek letter Delta.The main difference between the Delta interferometer and other existing interferometers,such as Michelson,Mach-Zehnder and Young's double-slit interferometers,is that the two interfering paths are asymmetrical in the Delta interferometer.The visibility of the first-order interference pattern observed in the Delta interferometer is dependent on the polarization of the incidental light.Optical coherence theory is employed to interpret this phenomenon and single-mode continuous-wave laser light is employed to verify the theoretical predictions.The theoretical and experimental results are consistent.The Delta interferometer is a perfect tool to study the reflection of electromagnetic fields in different polarizations and may find applications in polarization-sensitive scenarios.

关键词： phase sensitive interferometer Fresnel formula first-order interference

Transcriptomics and physiological analyses reveal that sulfur alleviates mercury toxicity in rice(Oryza sativa L.)

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Journal of Environmental Sciences 2024年第1期135卷 10-25页

作者： Yingmei Huang Jicai Yi Xiaomin Li Fangbai Li National-Regional Joint engineering Research center for Soil Pollution control and Remediation in South China Guangdong Key Laboratory of Integrated Agro-Environmental Pollution Control and ManagementInstitute of Eco-Environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China Guangzhou Institute of Geochemistry Chinese Academy of SciencesGuangzhou 510640China University of Chinese Academy of Sciences Beijing 100049China College of Life Sciences South China Agricultural UniversityGuangzhou 510642China SCNU Environmental Research Institute Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety&MOE Key Laboratory of Theoretical Chemistry of EnvironmentSouth China Normal UniversityGuangzhou 510006China

Mercury(Hg)is one of the most dangerous contaminants and has sparked global concern since it poses a health risk to humans when consumed through rice.Sulfur(S)is a crucial component for plant growth,and S may reduce Hg accumulation in rice grains.However,the detailed effects of S and the mechanisms underlying S-mediated responses in Hg-stressed rice plants remain unclear.Currently,to investigate the effects of S addition on rice growth,Hg accumulation,physiological indexes,and gene expression profiles,rice seedlings were hydroponically treated with Hg(20μmol/L Hg Cl_(2))and Hg plus elemental sulfur(100 mg/L).S application significantly reduced Hg accumulation in Hg-stressed rice roots and alleviated the inhibitory effects of Hg on rice growth.S addition significantly reduced Hg-induced reactive oxygen species generation,membrane lipid peroxidation levels,and activities of antioxidant enzymes while increasing glutathione content in leaves.Transcriptomic analysis of roots identified 3,411,2,730,and 581 differentially expressed genes in the control(CK)vs.Hg,CK vs.Hg+S,and Hg vs.Hg+S datasets,respectively.The pathway of S-mediated biological metabolism fell into six groups:biosynthesis and metabolism,expression regulation,transport,stimulus response,oxidation reduction,and cell wall biogenesis.The majority of biological process-related genes were upregulated under Hg stress compared with CK treatment,but downregulated in the Hg+S treatment.The results provide transcriptomic and physiological evidence that S may be critical for plant Hg stress resistance and will help to develop strategies for reduction or phytoremediation of Hg contamination.

关键词： Sulfur Mercury Transcriptomics Detoxification

Atomic Dispersed Hetero‑Pairs for Enhanced Electrocatalytic CO_(2)Reduction

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Nano-Micro Letters 2024年第1期16卷 55-67页

作者： Zhaoyong Jin Meiqi Yang Yilong Dong Xingcheng Ma Ying Wang Jiandong Wu Jinchang Fan Dewen Wang Rongshen Xi Xiao Zhao Tianyi Xu Jingxiang Zhao Lei Zhang David J.Singh Weitao Zheng Xiaoqiang Cui State Key Laboratory of Automotive Simulation and control School of Materials Science and EngineeringKey Laboratory of Automobile Materials of MOEElectron Microscopy CenterJilin UniversityChangchun 130012People’s Republic of China Key Laboratory of Photonic and Electronic Bandgap Materials Ministry of Educationand College of Chemistry and Chemical EngineeringHarbin Normal UniversityHarbin 150025People’s Republic of China College of Chemistry Jilin UniversityChangchun 130012People’s Republic of China Department of Physics and Astronomy and Department of Chemistry University of MissouriColumbiaMO 65211USA

Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,increasing the binding of the*COOH to the active site will generally increase the*CO desorption energy.Breaking this relationship may be expected to dramatically improve the intrinsic activity of CO_(2)RR,but remains an unsolved challenge.Herein,we addressed this conundrum by constructing a unique atomic dispersed hetero-pair consisting of Mo-Fe di-atoms anchored on N-doped carbon carrier.This system shows an unprecedented CO_(2)RR intrinsic activity with TOF of 3336 h−1,high selectivity toward CO production,Faradaic efficiency of 95.96%at−0.60 V and excellent stability.Theoretical calculations show that the Mo-Fe diatomic sites increased the*COOH intermediate adsorption energy by bridging adsorption of*COOH intermediates.At the same time,d-d orbital coupling in the Mo-Fe di-atom results in electron delocalization and facilitates desorption of*CO intermediates.Thus,the undesirable correlation between these steps is broken.This work provides a promising approach,specifically the use of di-atoms,for breaking unfavorable relationships based on understanding of the catalytic mechanisms at the atomic scale.

关键词： CO_(2)reduction reaction Atomic dispersed catalyst Hetero-diatomic pair Ad-desorption energy Linear scaling relation

Building Feedback-Regulation System Through Atomic Design for Highly Active SO_(2)Sensing

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Nano-Micro Letters 2024年第7期16卷 343-357页

作者： Xin Jia Panzhe Qiao Xiaowu Wang Muyu Yan Yang Chen Bao-Li An Pengfei Hu Bo Lu Jing Xu Zhenggang Xue Jiaqiang Xu NEST Lab Department of ChemistryCollege of SciencesShanghai UniversityShanghai 200444People’s Republic of China Shanghai Synchrotron Radiation Facility Zhangjiang LabShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204People’s Republic of China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026People’s Republic of China Key Laboratory of Organic Compound Pollution control engineering(moe) School of Environmental and Chemical EngineeringShanghai UniversityShanghai 200444People’s Republic of China Shanghai University Instrumental Analysis&Research Center of Shanghai UniversityShanghai 200444People’s Republic of China

Reasonably constructing an atomic interface is pronouncedly essential for surface-related gas-sensing reaction.Herein,we present an ingen-ious feedback-regulation system by changing the interactional mode between single Pt atoms and adjacent S species for high-efficiency SO_(2)sensing.We found that the single Pt sites on the MoS_(2)surface can induce easier volatiliza-tion of adjacent S species to activate the whole inert S plane.Reversely,the activated S species can provide a feedback role in tailoring the antibonding-orbital electronic occupancy state of Pt atoms,thus creating a combined system involving S vacancy-assisted single Pt sites(Pt-Vs)to synergistically improve the adsorption ability of SO_(2)gas molecules.Further-more,in situ Raman,ex situ X-ray photoelectron spectroscopy testing and density functional theory analysis demonstrate the intact feedback-regulation system can expand the electron transfer path from single Pt sites to whole Pt-MoS_(2)supports in SO_(2)gas atmosphere.Equipped with wireless-sensing modules,the final Pt1-MoS_(2)-def sensors array can further realize real-time monitoring of SO_(2)levels and cloud-data storage for plant growth.Such a fundamental understanding of the intrinsic link between atomic interface and sensing mechanism is thus expected to broaden the rational design of highly effective gas sensors.

关键词： Feedback-regulation system Atomic interface SO_(2)sensor Single-atom sensing mechanism Intelligent-sensing array

深低温保存下高效抗冻多肽的合理设计和机理探讨

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engineering 2024年第3期34卷 164-173页

作者： Haishan Qi Yihang Gao Lin Zhang Zhongxin Cui Xiaojie Sui Jianfan Ma Jing Yang Zhiquan Shu Lei Zhang Department of Biochemical engineering School of Chemical Engineering and TechnologyFrontier Science Center for Synthetic Biology and Key Laboratory of Systems Bioengineering(MOE)Tianjin UniversityTianjin 300350China School of engineering and Technology University of Washington TacomaTacomaWA 98402USA

The development of effective antifreeze peptides to control ice growth has attracted a significant amount of attention yet still remains a great challenge.Here,we propose a novel design method based on in-depth investigation of repetitive motifs in various ice-binding proteins(IBPs)with evolution analysis.In this way,several peptides with notable antifreeze activity were developed.In particular,a designed antifreeze peptide named AVD exhibits ideal ice recrystallization inhibition(IRI),solubility,and biocompatibility,making it suitable for use as a cryoprotective agent(CPA).A mutation analysis and molecular dynamics(MD)simulations indicated that the Thr6 and Asn8 residues of the AVD peptide are fundamental to its ice-binding capacity,while the Ser18 residue can synergistically enhance their interaction with ice,revealing the antifreeze mechanism of AVD.Furthermore,to evaluate the cryoprotection potential of AVD,the peptide was successfully employed for the cryopreservation of various cells,which demonstrated significant post-freezing cell recovery.This work opens up a new avenue for designing antifreeze materials and provides peptide-based functional modules for synthetic biology.

关键词： Antifreeze peptides Evolution analysis Ice recrystallization inhibition Molecular dynamics simulation Cryopreservation Synthetic biology