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Light-driven directional ion transport for enhanced osmotic energy harvesting

National Science Review 2021年第8期8卷 178-185页

作者： Kai Xiao Paolo Giusto Fengxiang chen Ruotian Chen Tobias Heil Shaowen Cao Lu chen Fengtao Fan Lei Jiang Max Planck Institute of Colloids and Interfaces Department of Colloid Chemistry Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education School of ChemistryBeihang University State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University State Key Laboratory of Catalysis 2011-iChEMDalian National Laboratory for Clean Energy (DNL)Dalian Institute of Chemical Physics(DICP)Chinese Academy of Sciences State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology

Light-driven ion(proton) transport is a crucial process both for photosynthesis of green plants and solar energy harvesting of some archaea. Here, we describe use of a TiO2/C3N4semiconductor heterojunction nanotube membrane to realize similar light-driven directional ion transport performance to that of biological systems. This heterojunction system can be fabricated by two simple deposition steps. Under unilateral illumination, the TiO2/C3N4heterojunction nanotube membrane can generate a photocurrent of about 9 μA/cm~2, corresponding to a pumping stream of ～5500 ions per second per nanotube. By changing the position of TiO2and C3N4, a reverse equivalent ionic current can also be realized. Directional transport of photogenerated electrons and holes results in a transmembrane potential, which is the basis of the light-driven ion transport phenomenon. As a proof of concept, we also show that this system can be used for enhanced osmotic energy generation. The artificial light-driven ion transport system proposed here offers a further step forward on the roadmap for development of ionic photoelectric conversion and integration into other applications, for example water desalination.

关键词： ion pump ion transport nanofluidic porous membrane carbon nitride

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Tailoring morphology symmetry of bismuth vanadate photocatalysts for efficient charge separation

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Science China Chemistry 2023年第12期66卷 3611-3619页

作者： Yuting Deng Hongpeng Zhou chenwei Ni Fengke Sun Wenchao Jiang Ruotian Chen Wenming Tian Can Li Rengui Li State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China State Key Laboratory of Molecular Reaction Dynamics and the Dynamic Research Center for Energy and Environmental Materials Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Although spatial charge separation between different facets of semiconductor crystals has been recognized as a general strategy in photocatalysis, the vital role of crystal morphology symmetry in charge separation properties still remains elusive. Herein,taking monoclinic bismuth vanadate(BiVO_(4)) as a platform, we found distinct charge separation difference via rationally tailoring the morphology symmetry from octahedral to truncated octahedral crystals. For octahedral BiVO_(4), photogenerated electrons and holes can be separated between edges and quasi-equivalent facets. However, as for truncated octahedral crystals,photogenerated electrons tend to transfer to {010} facets while photogenerated holes prefer to accumulate on {120} facets, thus realizing the spatial separation of photogenerated charge between different facets. Morphology tailoring of BiVO_(4) crystals leads to a significantly improved photogenerated charge separation efficiency and photocatalytic water oxidation activity. The built-in electric field for driving the separation of photogenerated electrons and holes is considered to be modulated by tuning the morphology symmetry of BiVO_(4) crystals. This work discloses the significant roles of morphology symmetry in photogenerated charge separation and facilitates the rational design of artificial photocatalysts.

关键词： bismuth vanadate morphology symmetry tailoring photocatalysis spatial charge separation

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Visualizing the role of applied voltage in non-metal electrocatalysts

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National Science Review 2023年第9期10卷 46-55页

作者： Ziyuan Wang Jun chen chenwei Ni Wei Nie Dongfeng Li Na Ta Deyun Zhang Yimeng Sun Fusai Sun Qian Li Yuran Li Ruotian Chen Tiankai Bu Fengtao Fan Can Li Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of Sciences 2. Department of ChemistryCollaborative Innovation Center of Chemistry for Energy Materials (iChEM)College of Chemistry and Chemical Engineering Xiamen University Energy College University of Chinese Academy of Sciences Department of Materials Imperial College London

Understanding how applied voltage drives the electrocatalytic reaction at the nanoscale is a fundamental scientific problem,particularly in non-metallic electrocatalysts,due to their low intrinsic carrier concentration.Herein,using monolayer molybdenum disulfide(MoS2) as a model system of non-metallic catalyst,the potential drops across the basal plane of MoS2(△Vsem) and the electric double layer(△Vedl)are decoupled quantitatively as a function of applied voltage through in-situ surface potential microscopy.We visualize the evolution of the band structure under liquid conditions and clarify the process of EFkeeping moving deep into Ec, revealing the formation process of the electrolyte gating effect.Additionally,electron transfer(ET) imaging reveals that the basal plane exhibits high ET activity,consistent with the results of surface potential measurements.The potential-dependent behavior of kfand nsin the ET reaction are further decoupled based on the measurements of △Vsemand △Vedl.Comparing the ET and hydrogen evolution reaction imaging results suggests that the low electrocatalytic activity of the basal plane is mainly due to the absence of active sites,rather than its electron transfer ability.This study fills an experimental gap in exploring driving forces for electrocatalysis at the nanoscale and addresses the long-standing issue of the inability to decouple charge transfer from catalytic processes.

关键词： non-metal electrocatalyst surface potential electron transfer hydrogen evolution reaction mapping

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Tip-induced directional charge separation on one-dimensional BiVO4 nanocones for asymmetric light absorption

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Journal of Energy Chemistry 2022年第9期31卷 326-332,I0009页

作者： Nengcong Yang Ruotian Chen chenwei Ni Dongfeng Li Qi Sun Lifang Liu Yu Qi Shengye Jin Xiuli Wang Fengtao Fan Can Li Fuxiang Zhang State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsDalian National Laboratory for Clean EnergyChinese Academy of SciencesDalian 116023LiaoningChina State Key Laboratory of Molecular Reaction Dynamics and Dynamics Research Center for Energy and Environmental Materials Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

One dimensional(1D)semiconductor is a class of extensively attractive materials for many emerging solar energy conversion technologies.However,it is still of shortage to assess the impact of 1D structural symmetry on spatial charge separation and understand its underlying mechanism.Here we take controllably-synthesized 1D BiVO_(4)nanocones and nanorods as prototypes to study the influence of 1D symmetry on charge separation.It is found that the asymmetric BiVO_(4)nanocones enable more effective charge separation compared with the symmetric nanorods.The unexpected spatial charge separation on the nanocones is mainly ascribed to uneven light absorption induced diffusion-controllable charge separation due to symmetry breaking of 1D nanostructure,as evidenced by spatial and temporal resolved spectroscopy.Moreover,the promotion effect of charge separation on the nanocones was quantitatively evaluated to be over 20 times higher than that in BiVO_(4)nanorods.This work gives the first demonstration of the influence of 1D structural symmetry on the charge separation behavior,providing new insights to design and fabricate semiconductor materials for efficient solar energy conversion.

关键词： Charge separation Tip-enhanced light absorption Surface photovoltage BiVO4 Photocatalysis

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Probing of coupling effect induced plasmonic charge accumulation for water oxidation

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National Science Review 2021年第6期8卷 160-168页

作者： Yuying Gao Feng cheng Weina Fang Xiaoguo Liu Shengyang Wang Wei Nie Ruotian Chen Sheng Ye Jian Zhu Hongyu An Chunhai Fan Fengtao Fan Can Li State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyCollaborative Innovation Center of Chemistry for Energy Materials (i Ch EM)Dalian Institute of Chemical PhysicsChinese Academy of Sciences University of Chinese Academy of Sciences School of Chemistry and Chemical Engineering and Institute of Molecular MedicineRenji HospitalSchool of MedicineShanghai Jiao Tong University

A key issue for redox reactions in plasmon-induced photocatalysis, particularly for water oxidation, is the concentration of surface-accumulating charges(electrons or holes) at a reaction site for artificial photosynthesis. However, where plasmonic charge accumulated at a catalyst’s surface, and how to improve local charge density at active sites, remains unknown because it is difficult to identify the exact spatial location and local density of the plasmon-induced charge, particularly with regard to holes. Herein, we show that at the single particle level, plasmon-coupling-induced holes can be greatly accumulated at the plasmonic Au nanoparticle dimer/Ti O2 interface in the nanogap region, as directly evidenced by the locally enhanced surface photovoltage. Such an accumulation of plasmonic holes can significantly accelerate the water oxidation reaction(multi-holes involved) at the interfacial reaction site, with nearly one order of magnitude enhancement in photocatalytic activities compared to those of highly dispersed Au nanoparticles on Ti O2. Combining Kelvin probe force microscopy and theoretical simulation, we further clarified that the local accumulated hole density is proportional to the square of the local near-field enhancement. Our findings advance the understanding of how charges spatially distribute in plasmonic systems and the specific role that local charge density at reaction sites plays in plasmonic photocatalysis.

关键词： plasmonic photocatalysis coupling effect charge separation surface photovoltage spatial distribution

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Formation of multifaceted nano-groove structure on rutile TiO_(2) photoanode for efficient electron-hole separation and water splitting

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Journal of Energy Chemistry 2022年第2期31卷 19-25页

作者： Xiaoyi Zhan Yaling Luo Ziyu Wang Yao Xiang Zheng Peng Yong Han Hui Zhang Ruotian Chen Qin Zhou Hongru Peng Hao Huang Weimin Liu Xin Ou Guijun Ma Fengtao Fan Fan Yang Can Li Zhi Liu State Key Laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050China School of Physical Science and Technology Shanghai Tech UniversityShanghai 201210China State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Photoelectrochemical(PEC)water-splitting using solar energy holds great promise for the renewable energy future,and a key challenge in the development of industry viable PEC devices is the unavailability of high-efficient photoanodes.Herein,we designed a TiO_(2) model photocatalyst with nano-groove pattern and different surface orientation using low-energy Ar+irradiation and photoetching of TiO_(2),and significantly improved the intrinsic activity for PEC water oxidation.High-resolution transmission electron microscopy directly manifests that the grooves consist of highly stepped surface withsteps and well-crystallized.Transient absorption spectroscopy reveals the groove surface that allows for increased recovery lifetime,which ensures promoted electron-hole separation efficiency.Surface photovoltage directly shows the carrier separation and transportation behaviors,verified by selective photodeposition,demonstrating the groove surface on TiO_(2) contributes to electron-hole separation.This work proposes an efficient and scalable photoanode strategy,which potentially can open new opportunities for achieving efficient PEC water oxidation performance.

关键词： TiO_(2)nano-grooves Oxygen vacancies Photoetching Water oxidation

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JGJ/T 441—2019中人致楼盖结构动力响应反应谱方法详解与实例对比

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土木工程学报 2023年第12期56卷 1-7,20页

作者：陈隽娄宇吕佐超徐若天同济大学上海200092 中国电子工程设计院有限公司北京100142 北京市微振动环境控制工程技术研究中心北京100142 华东建筑设计研究院有限公司上海200002

大跨度、开敞式、轻质建筑楼盖的大量使用以及用户体验满意度要求的不断提高,使得人致荷载下的楼盖振动舒适度问题日益突出,也已成为大跨楼盖结构设计的关键问题。为此,中国电子工程设计院有限公司联合多单位编制了《建筑楼盖结构振动... 详细信息

大跨度、开敞式、轻质建筑楼盖的大量使用以及用户体验满意度要求的不断提高,使得人致荷载下的楼盖振动舒适度问题日益突出,也已成为大跨楼盖结构设计的关键问题。为此,中国电子工程设计院有限公司联合多单位编制了《建筑楼盖结构振动舒适度技术标准》(JGJ/T 441—2019),并已于2020年1月1日起实施。文章针对《标准》中单人步行荷载下楼盖结构响应的反应谱计算方法,详细说明了其理论基础、简化依据和计算步骤。进而,将反应谱方法应用于50个已建钢-混凝土组合结构楼盖、3个已建混凝土楼盖、1个木楼盖试验模型、1个已建人行桥和英国设计标准中2个范例的人致结构振动分析与舒适度评估,并与上述例子的实测值或标准计算值进行了比较。对比结果显示了反应谱方法对多类型结构人致振动分析的适用性,同时也进一步明确了阻尼比、模态质量等关键计算参数的选取原则以及反应谱方法的使用范围。

关键词：振动舒适度大跨度楼盖反应谱方法人致荷载技术标准

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The increasing expression of GPX7 related to the malignant clinical features leading to poor prognosis of glioma patients

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Chinese Neurosurgical Journal 2021年第2期7卷 107-115页

作者： Jiawei Yao Xin chen Zhendong Liu ruotian Zhang cheng Zhang Quan Yang Penglei Yao Qiuyi Jiang Jianing Wu Shiguang Zhao Department of Neurosurgery First Affiliated Hospital of Harbin Medical UniversityNo.23 Youzheng StreetNangang DistrictHarbin 150001Heilongjiang ProvinceChina Key Colleges and Universities Laboratory of Neurosurgery in Heilongjiang Province Harbin 150001Heilongjiang ProvinceChina Department of Neurosurgery The Pinghu Hospital of Shenzhen UniversityShenzhen 518100Guangdong ProvinceChina Institute of Neuroscience Sino-Russian Medical Research CenterHarbin Medical UniversityHarbin 150001Heilongjiang ProvinceChina North Broward Preparatory School 7600 Lyons RdCoconut CreekFL 33073USA

Background:Glioma is the most common malignant brain tumor in adults.The standard treatment scheme of glioma is surgical resection combined alternative radio-and chemotherapy.However,the outcome of glioma patients was unsatisfied.Here,we aimed to explore the molecular and biological function characteristics of GPX7 in glioma.Methods:The multidimensional data of glioma samples were downloaded from Chinese Glioma Genome Atlas(CGGA).RT-qPCR method was used to identify the expression status of GPX7.Kaplan–Meier curves and Cox regression analysis were used to explore the prognostic value of GPX7.Gene Set Enrichment Analysis(GSEA)was applied to investigate the GPX7-related functions in glioma.Results:The results indicated that the expression of GPX7 in glioma was higher compared to that in normal brain tissue.Univariate and multivariate Cox regression analyses confirmed that the expression value of GPX7 was an independent prognostic factor in glioma.The GSEA analysis showed that GPX7 was significantly enriched in the cell cycle pathway,ECM pathway,focal adhesion pathway,and toll-like receptor pathway.Conclusions:The GPX7 was recommended as an independent risk factor for patients diagnosed with glioma for the first time and GPX7 could be potentially used as the therapy target in future.Furthermore,we attempted to explore a potential biomarker for improving the diagnosis and prognosis of patients with glioma.

关键词： GPX7 Glioma Biomarker Survival

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Long-time exposure of general anesthetics impairs astrocyte morphology and Ca2+ signaling in developing mouse brain

Long-time exposure of general anesthetics impairs astrocyte ...

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中国神经科学学会第十二届全国学术会议

作者： Bin Zhou Lingmin chen Zhenpeng Song ruotian Jiang Department of Anesthesiology West China Hospital Sichuan University Translational Neuroscience Center West China Hospital Sichuan University

Objective Cautions should be taken when long-time or multiple exposures of general anesthetics are applied in children under 3 years old, as suggested by the FDA of USA. Indeed, studies in rodents and primates indicate that such procedure results in neuronal dysfunctions/apoptosis and cognitive decline. Astrocytes are vital for synaptic growth and circuitry formation in the developing brain;however, the involvement of astrocytes in anesthetics-induced developmental neurotoxicity(AIDN) remains largely unknown. The aim of the present study is to evaluate the toxic effects of long-time exposure of sevoflurane, a commonly used general anesthetics in pediatrics, on developing astrocytes in mice, and to reveal glial mechanisms for AIDN. Methods After exposure of sevoflurane(Sevo) or carrier gas(control) for 4 h, individual cortical astrocyte in brain slices from neonate mice(P7) was fluorescently labeled using iontophresis with lucifer yellow. Morphological 3 D reconstructions were performed using high-resolution confocal microscopy, and were analyzed using the software Imaris. The acute and chronic effects of sevoflurane on astrocyte Ca signaling were assessed using confocal imaging in brain slices with GCaMP6 f selectively expressed in astrocytes. Results The volume of cortical astrocyte territory, branchlets, and proximal/peripheral fine processes in Sevo group were markedly decreased when assessed 12 h and 7 days(P14) after exposure. Chronic effects of Sevo in astrocyte Ca are complex in multiple levels, which involve store-mediated Ca and extracellular Ca disturbance. The acute application of Sevo induced a decrease of astrocyte basal Ca level. Conclusion Longtime exposure of sevoflurane leads to impaired morphological development associated with dysfunctional Ca signaling in cortical astrocytes during the peak period of synaptogensis. How the observed astrocyte deficits contribute to AIND is under investigation.

关键词： general anesthetics neurotoxicity development astrocytes

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Roles of astrocytic two-pore domain potassium channels in cerebral focal ischemia

Roles of astrocytic two-pore domain potassium channels in ce...

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中国神经科学学会第十二届全国学术会议

作者： Lingmin chen Bin Zhou Zhenpeng Song ruotian Jiang Department of Anesthesiology and 2Translational Neuroscience Center West China Hospital Sichuan University

Objective Suppressing astrocyte-mediated glutamate release and intervening its ion homeostatic functions during cerebral focal ischemia reduce neural damage. Nevertheless, the key membrane protein(s) regulating glutamate release and ion homeostasis within astrocytes during ischemia remains unidentified. The present study is to explore the key roles of astrocytic two-pore domain potassium channels TWIK1 and TREK1 in regulating glutamate and ion homeostasis in mouse models of ischemia. Methods Acute brain slice patch-clamp electrophysiology and confocal imaging with genetically encoded glutamate indicator i GluSnFR were used to monitor astrocyte glutamate release, and GCaMP6f was used to image astrocyte calcium signals, in brain slices after oxygen glucose deprivation(OGD) or from mice subjected to middle cerebral artery occlusion(MCAO). CRISPR-Cas9 technique was used to manipulate TWIK1/TREK1 knockout within astrocytes. Results(1) Slow inward currents(SICs) were recorded in cortical pyramidal neurons after OGD in the presence of TTX and Cd, suggesting a non-neuronal glutamate source released onto neurons.(2) Spontaneous i Glu Sn FR signals were recorded within astrocyte territories, suggesting astrocyte glutamate release, and they were largely inhibited by quinine, a two-pore K channel inhibitor.(3) Astrocytes spontaneous Ca signals were significantly increased after OGD, and they were largely inhibited by quinine. Conclusion Two-pore domain potassium channel TWIK1/TREK1 were likely involved in astrocyte-mediated glutamate release and astrocyte Ca dysfunctions during brain ischemia. The underlying release mechanisms and the Ca-dependent release pathways are currently under investigation using astrocytic TWIK1/TREK1 knockout mice.

关键词： astrocytes two-pore domain potassium channels ischemia glutamate excitoxicity Ca2+ homeostasis

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