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Bias distribution and regulation in photoelectrochemical overall water-splitting cells

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National Science Review 2024年第4期11卷 141-150页

作者： Kun Dang Siqin Liu Lei Wu Daojian Tang Jing Xue Jiaming Wang Hongwei Ji Chuncheng Chen Yuchao Zhang Jincai Zhao key {1. of photochemistry CAS ResearchEducation Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences University of Chinese Academy of Sciences

The water oxidation half-reaction at anodes is always considered the rate-limiting step of overall water splitting（OWS）,but the actual bias distribution between photoanodes and cathodes of photoelectro chemical（PEC） OWS cells has not been investigated *** this work,we find that,for PEC cells consisting of photoanodes（nickel-modified n-Si [Ni/n-Si] and α-Fe2O3） with low photovoltage(Vph1.V),a large portion of applied bias is exerted on the Pt cathode for satisfying the hydrogen evolution thermodynamics,showing a thermodynamics-controlled *** contrast,for photoanodes（TiO2and BiVO4） with Vph> 1.,the bias required for cathode activation can be significantly reduced,exhibiting a kinetics-controlled *** investigations show that the bias distribution can be regulated by tuning the electrolyte pH and using alternative half-reaction ***,a volcano plot is presented for the rational design of the overall reactions and unbiased PEC *** by this,an unbiased PEC cell consisting of a simple Ni/n-Si photoanode and Pt cathode is assembled,delivering a photo current density of 5.3±0.2 mA cm-2.

关键词： photoelectrochemistry overall reaction cell bias distribution photoanode water splitting

A review on plasmonic enhancement of activity and selectivity in electrocatalytic CO_(2)reduction

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Frontiers in Energy 2024年第4期18卷 399-417页

作者： Jing XUE Zhenlin CHEN Yuchao ZHANG Jincai ZHAO key {1. of photochemistry Beijing National Laboratory for Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Utilizing plasmonic effects to assist electrochemical reactions exhibits a huge potential in tuning the reaction activities and product selectivity,which is most appealing especially in chemical reactions with multiple products,such as CO_(2)reduction reaction(CO_(2)RR).However,a comprehensive review of the development and the underlying mechanisms in plasmon-assisted electrocatalytic CO_(2)RR remains few and far ***,the fundamentals of localized surface plasmonic resonance(LSPR)excitation and the properties of typical plasmonic metals(including Au,Ag,and Cu)are ***,the potential mechanisms of plasmonic effects(such as hot carrier effects and photothermal effects)on the reaction performance in the field of plasmon-assisted electrocatalytic CO_(2)RR are summarized,which provides directions for the future development of this *** is concluded that plasmonic catalysts exhibit potential capabilities in enhancing CO_(2)RR while more in situ techniques are essential to further clarify the inner mechanisms.

关键词： localized surface plasmonic resonance(LSPR)effect plasmonic metals CO_(2)reduction reaction(CO_(2)RR) hot carrier effect photothermal effect

Acceptor-Type Singlet Fission Material Based on Strong Absorption Tetracyanothienoquinoid Skeleton

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CCS Chemistry 2024年第9期6卷 2142-2149页

作者： Senhao Wang Xiang-Yang Liu Mengfan Zhang Long Wang Ganglong Cui Hongbing Fu Jiannian Yao key {1. of Interface Science and Engineering in Advanced Materials Ministry of EducationTaiyuan University of TechnologyTaiyuan 030024 College of Chemistry and Material Science Sichuan Normal UniversityChengdu 610068 key {1. of Theoretical and Computational photochemistry Ministry of EducationCollege of ChemistryBeijing Normal UniversityBeijing 100875 Beijing key {1. for Optical Materials and Photonic Devices Department of ChemistryCapital Normal UniversityBeijing 100048 Beijing National laboratory for Molecules Science(BNLMS) Key Laboratory of PhotochemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190

The practical efficiency of singlet fission(SF)-based photovoltaic devices is still far from satisfactory due to the limited scope of SF materials suitable for device application and the scarcity of schemes available for triplet *** SF materials identi-fied to date are typically electron donors while acceptor-type SF materials remain largely ***,the combination of a conventional electron donor and SF-active electron acceptor could circumvent the competitive energy transfer channel and better play the unique advantages of the SF process,which might be an adequate alternative for practical *** this work,we presented a new acceptor-type SF material based on a tetracyanothienoquinoid *** a quinoid skeleton exhibited strong absorption,ultrafast SF process,and excellent *** transient spectroscopy and multireference calculations(XDWCASPT2),the SF dynamics were examined featuring the rapid generation and subsequent annihilation and/or partial dissociation of multiexciton ***,our results not only provide a robust acceptor-type SF material but also suggest an adequate donor–acceptor alternative for SF-based solar cells,which could pave the way for the practical application of such a potential process.

关键词： singlet fission acceptor quinoidal skeleton mutiexciton state multireference calculation transient spectroscopy

Triplet-triplet annihilation upconversion materials as electrophoretic inks

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Chinese Chemical Letters 2024年第3期35卷 439-442页

作者： Qiaoyu Zhang Guiwen Luo Jinping Chen Tianjun Yu Rui Hu Guoqiang Yang Yi Zeng Yi Li key {1. of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China key {1. of photochemistry Institute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Luminescent materials that can be reversibly switched by electric field stimulation are attractive since the potential application for optoelectronic *** we report a triplet-triplet annihilation upconversion(TTA-UC)system with electrophoretic response which is developed as the electrophoretic *** TTA-UC system consists of an ionic derivative of 9,1.-diphenyl anthracene(DPA)as the annihilator and Pt(II)octaethylporphyrin(PtOEP)as the *** applying an electric field,migration and enrichment of positively charged DPA derivatives towards the cathode results in a 20%enhancement of TTA-UC.A quasi-solid film for electrically writing is made using the electrophoretic TTA system as the ink and a platinum electrode as a *** prototype of TTA-UC ink demonstrates unique luminescence functions upon electrically writing and erasing,providing a promising strategy to develop electronic devices for display,information storage and encryption.

关键词： Triplet-triplet annihilation Photon upconversion Electrophoresis Electrophoretic ink Luminescence display

Asymmetric radical allylation of β-keto esters with vinyl cyclopropanes by dual photoredox/nickel catalysis

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Science China Chemistry 2024年第11期67卷 3807-3816页

作者： Wen-Yuan Qu Xue-Song Zhou Wen-Jing Xiao Jia-Rong Chen Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction Ministry of EducationCollege of Chemistry Central China Normal University Wuhan Institute of photochemistry and Technology key {1. of Organo-Pharmaceutical Chemistry of Jiangxi Province Gannan Normal University

Radical-involved allylation reactions have emerged as a powerful platform for construction of carbon-carbon and carbonheteroatom bonds, facilitating the strategic incorporation of diverse allyl moieties. Nevertheless, this burgeoning field still faces ongoing challenges, including limitations of radical precursors and coupling partners, and difficulties in achieving enantiocontrol. Herein, we report for the first time a highly enantioselective radical allylation involving β-keto esters with vinyl cyclopropanes utilizing a synergistic dual photoredox/nickel catalysis under visible light irradiation. The mild and redox-neutral catalytic protocol demonstrates an extensive substrate compatibility and good functional tolerance, providing access to enantioenriched β-keto esters featuring quaternary α-stereocenter with good yields and high enantioselectivities. Preliminary mechanistic studies have uncovered that the success of the reaction hinges on the dual roles of nickel catalyst, including in situ formation of photoredox sensitive substrate/Ni complex and the ensuing asymmetric radical addition step.

关键词： asymmetric allylation photoredox catalysis radical addition nickel catalysis β-keto esters vinyl cyclopropanes

Nitrogen-doping boosts *CO utilization and H2O activation on copper for improving CO2 reduction to C2+ products

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Green Energy & Environment 2024年第9期9卷 1459-1465页

作者： Yisen Yang Zhonghao Tan Jianling Zhang Jie Yang Renjie Zhang Sha Wang Yi Song Zhuizhui Su Beijing National laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences School of Chemical Sciences University of Chinese Academy of Sciences key {1. of photochemistry CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences

To improve the electrocatalytic transformation of carbon dioxide （CO2） to multi-carbon (C2+) products is of great *** we developed a nitrogen-doped Cu catalyst,by which the maximum C2+Faradaic efficiency can reach 72.7%in flow-cell system,with the partial current density reaching 0.62 A *** in situ Raman spectra demonstrate that the *CO adsorption can be strengthened on such a N-doped Cu catalyst,thus promoting the*CO utilization in the subsequent C–C coupling ***,the water activation can be well enhanced by N doping on Cu *** to the synergistic effects,the selectivity and activity for C2+products over the N-deoped Cu catalyst are much improved.

关键词： Electrocatalytic CO 2 reduction reaction Copper catalyst Doping Multi-carbon products In situ Raman measurement

Single-atom Ni-N_(4) for enhanced electrochemical sensing

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Nano Research 2024年第8期17卷 7658-7664页

作者： Zhuhui Qin Bo Tang Guiru Zhang Chongqing Zhu Kun Jiang Bowei Zhang Fu-Zhen Xuan Shanghai key {1. of Intelligent Sensing and Detection Technology East China University of Science and TechnologyShanghai 200237China key {1. of Pressure Systems and Safety of Ministry of Education East China University of Science and TechnologyShanghai 200237China School of Mechanical and Power Engineering East China University of Science and TechnologyShanghai 200237China key {1. of Theoretical and Computational photochemistry Ministry of EducationCollege of ChemistryBeijing Normal UniversityBeijing 100875China Interdisciplinary Research Center School of Mechanical EngineeringShanghai Jiao Tong UniversityShanghai 200240China

Single-atom catalysts(SACs)attract widespread attention in heterogeneous catalysis due to their maximum atomic utilization efficiency and unique physical and chemical ***,their applications in chemical sensing keep huge potential but remain ***,a Ni-N_(4)-C SAC was synthesized for the trace detection of dopamine(DA)and uric acid(UA).The Ni-N_(4)-C SAC exhibited superior sensing performance compared to the Ni *** detection range for DA and UA were 0.05–75μM and 5–90μM with detection limits of 0.027 and 0.82μM,*** functional theory(DFT)computations indicate that Ni-N_(4)-C has a lower reaction barrier during electrochemical process,indicating that the atomic Ni sites possess higher intrinsic activity than Ni ***,DA and UA show strong potential dependency on the Ni-N_(4)-C catalyst,indicating its applicability for their concurrent *** work extends the application of SACs in chemical sensing.

关键词： single-atom catalysts chemical sensing dopamine uric acid

Approaches to Improving Selectivity During Photoelectrochemical Transformation of Small Molecules

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Transactions of Tianjin University 2024年第2期30卷 167-177页

作者： Sipeng Yang Jie Yang Mengyu Duan Shirong Kang Shaohua He Chuncheng Chen key {1. of photochemistry CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100190China

Photoelectrochemical (PEC) small-molecule oxidation can selectively transform substrates into high-value-added fine chemicals and increase the rate of cathode hydrogen evolution. Nevertheless, achieving high-selectivity PEC oxidation of small molecules to produce specific products is a very challenging task. In general, selectivity can be improved by changing the surface catalyticsites of the photoanode and modulating the interfacial environments of the reactions. Herein, recent advances in approaches to improving selective PEC oxidation of small molecules are introduced. We first briefly discuss the basic concept and fundamentals of small-molecule PEC oxidation. The reported approaches to improving the performance of selective PEC oxidation of small molecules are highlighted from two aspects: (1. changing the surface properties of photoanodes by selecting suitable materials or modifying the photoanodes and (2) mediating the oxidation reactions using redox mediators. The PEC oxidation mechanism of these studies is emphasized. We also discuss the challenges in this research direction and offer a perspective on the further development of selective PEC-based small-molecule transformation.

关键词： Photoelectrocatalytic Small-molecule oxidation Improving selectivity Surface properties Mediating

Fermi Rubik's Cube in High-Pressure Induced Chlorine-Rich Compounds

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Chinese Physics Letters 2024年第10期41卷 78-83页

作者： Jun Kong Lei Su Haixu Cui Hairui Ding Jingyu Hou Chunxia Chi Shiyang Liu Xiang-Feng Zhou Hui-Tian Wang Xiao Dong key {1. of Weak-Light Nonlinear Photonics and School of Physics Nankai UniversityTianjin 300071China Center for High Pressure Science and Technology Advanced Research Beijing 100093China key {1. of photochemistry Institute of ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesBeijing 100190China College of Physics and Materials Science Tianjin Normal UniversityTianjin 300387China Center for High Pressure Science State Key Laboratory of Metastable Materials Science and TechnologySchool of ScienceYanshan UniversityQinhuangdao 066004China National laboratory of Solid State Microstructures School of Physicsand Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210093China

In the quasi-free electron model,the Fermi surface spreads into a sphere in the Brillouin zone,i.e.,the Fermi *** Fermi sphere exists widely in metal systems,no matter whether the crystal is in a body-center cubic,face-center cubic,or hexagonal close-packed ***,we report a class of compounds stabilized at high pressure with Rubik’s cubic Fermi surface.

关键词： surface. Fermi cubic