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Ethanol-assisted synthesis of a Ni single-atom catalyst with poriferous 3D framework for efficient cascade CO2 electroreduction

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Rare Metals 2024年第9期43卷 4612-4619页

作者： Feng Wu Shi-Qi Wang Sebastian Kunze Xiao-Ping Gao Pei-Qun Yin Yu-En Wu Division of Life Sciences and Medicine Department of Endocrinology School of Chemistry and Materials Science The First Affiliated Hospital of USTC University of Science and Technology of China department of chemistry Seoul National University School of Biomedical Engineering Anhui Medical University

The electroreduction of carbon dioxide to generate multicarbon products is significant for achieving a carbon-neutral economy. However, the selectivity for multi-carbon products faces several challenges, such as the intricate nature of the multistep hydrogenation processes, slow reaction kinetics and the bicarbonate precipitate issue caused by alkaline conditions. These factors hinder the extensive utilization of this reaction. Herein, we successfully developed and implemented a tandem electrolyzer cascade to separate and optimize the complex elementary reactions involved in the process of multi-carbon production. This approach enables us to enhance the Faradaic efficiency (FE) of each step, consequently improving the overall performance of the system. An ethanol-assisted ionic-exchange method was utilized to synthesize a Ni

关键词： ELECTROCHEMICAL REDUCTION CARBON-DIOXIDE artificial photosynthesis OXYGEN REDUCTION ENERGY HYDROCARBONS COORDINATION CHALLENGES HYDROGEN ETHYLENE

Necessity of structural rearrangements for O-O bond formation between O5 and W2 in photosystemⅡ

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Journal of Energy chemistry 2021年第6期30卷 436-442,I0011页

作者： Yu Guo Biaobiao Zhang Lars Kloo Licheng Sun department of chemistry School of Engineering Sciences in ChemistryBiotechnology and HealthKTH Royal Institute of Technology.S E-10044 StockholmSweden State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT-KTH Joint Education and Research Center on Molecular DevicesDalian University of Technology(DUT)Dalian 116024LiaoningChina Center of artificial photosynthesis for solar fuels School of ScienceWestlake University.Hangzhou 310024ZhejiangChina

Numerous aspects of the water oxidation mechanism in photosystemⅡhave not been fully elucidated,especially the O-O bond formation ***,a body of experimental evidences have identified the O5 and W2 ligands of the oxygen-evolving complex as the highly probable substrate *** this work,we studied O-O bond formation between O5 and W2 based on the native Mn4 Ca cluster by density functional *** rearrangements before the formation of the S_(4) state were found as a prerequisite for O-O bond formation between O5 and W2,regardless if the suggested pathways involving the typical Mnl(Ⅳ)-O·species or the recently proposed Mn4(Ⅶ)(O)2 *** alternatives for the S2→S_(3) and S_(3)→S_(4) transitions accounting for such required rearrangements are *** findings reflect that the structural flexibility of the Mn4 Ca cluster is essential to allow structural rearrangements during the catalytic cycle.

关键词： Density functional theory Oxygen-evolving complex Substrate water OAO bond formation Structural rearrangement

2D materials for solar fuels via artificial photosynthesis

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National Science Review 2022年第5期9卷 19-21页

作者： Jian Du Hao Yang Licheng Sun Institute of Natural Sciences Westlake Institute for Advanced Study Center of artificial photosynthesis for solar fuels School of ScienceWestlake University department of chemistry School of Engineering Sciences in Chemistry Biotechnology and Health KTH Royal Institute of Technology State Key Laboratory of Fine Chemicals DUT-KTH Joint Education and Research Centre on Molecular Devices Dalian University of Technology

To create a globally carbon neutral society,sustainable energy systems to replace fossil fuels are needed *** in nature converts CO2and H2O into carbohydrates and O2and is driven by solar energy via photosystemⅡ(PSⅡ...

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Dye-sensitized photoanode decorated with pyridine additives for efficient solar water oxidation

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Chinese Journal of Catalysis 2021年第8期42卷 1352-1359页

作者： Jiayuan Li Yong Zhu Fei Li Guoquan Liu Suxian Xu Licheng Sun State Key Laboratory of Fine Chemicals DUT-KTH Joint Education and Research Center on Molecular DevicesDalian University of Technology(DUT)Dalian 116024LiaoningChina department of chemistry School of Engineering Sciences in ChemistryBiotechnology and HealthKTH Royal Institute of TechnologyStockholm 10044Sweden Center of artificial photosynthesis for solar fuels School of ScienceWestlake UniversityHangzhou 310024ZhejiangChina

Splitting water into hydrogen and oxygen by dye-sensitized photoelectrochemical cell(DSPEC)is a promising approach to solar fuels *** this study,a series of pyridine derivatives as surface additives were modified on a molecular chromophore and water oxidation catalyst co-loaded TiO_(2)photoanode,TiO_(2)|RuP,1(RuP=Ru(4,4′-(PO3H2)2-2,2′-bipyridine)(2,2′-bipyridine)2,1=Ru(bda)(L)2,(bda=2,2′-bipyridine-6,6′-dicarboxylate,L=10-(pyridin-4-yloxy)decyl)phosphonic acid).The addition of pyridine additives was found to result in up to 42%increase in *** simulated sun-light irradiation,TiO_(2)|RuP,1,P1(P1=4-Hydroxypyridine)produced a photocurrent density of 1 mA/cm2 at a bias of 0.4 V *** in acetate ***,the observed photocurrents are correlated with the electron-donating ability of the substituent groups on pyridine *** absorption measurements and electrochemical impedance spectroscopy revealed that surface-bound pyridine can effectively retard the back-electron transfer from the TiO_(2)conduction band to the oxidized dye,which is a major process responsible for energy loss in DSPECs.

关键词： Dye-sensitized photoelectrochemical cell Water splitting Photoanode Surface modification Pyridine derivatives

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A novel phenoxazine-based hole transport material for efficient perovskite solar cell

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Journal of Energy chemistry 2015年第6期24卷 698-706页

作者： Ming Cheng Cheng Chen Bo Xu Yong Hua Fuguo Zhang Lars Kloo Licheng Sun department of chemistry Organic ChemistryKTH Royal Institute of Technology department of chemistry Applied Physical ChemistryKTH Royal Institute of Technology State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT–KTH Joint Education and Research Centre on Molecular DevicesDalian University of Technology (DUT)

Based on the previous research work in our laboratory, we have designed and synthesized a small-molecule, hole transport material （HTM） POZ6-2 using phenoxazine （POZ） as central unit and dicyanovinyl units as electron-withdrawing terminal groups. Through the introduction ofa 2-ethyl-hexyl bulky chain into the POZ core unit, POZ6-2 exhibits good solubility in organic solvents. In addition, POZ6-2 possesses appropriate energy levels in combination with a high hole mobility and conductivity in its pristine form. Therefore, it can readily be used as a dopant-flee HTM in perovskite solar cells （PSCs） and a conversion efficiency of 10.3% was obtained. The conductivity of the POZ6-2 layer can be markedly enhanced via doping in combination with typical additives, such as 4-tert-butylpyridine （TBP） and lithium bis（trifluoromethanesulfonyl） imide （LiTFS1）. Correspondingly, the efficiency of the PSCs was further improved to 12.3% using doping strategies. Under the same conditions, reference devices based on the well-known HTM Spiro-OMeTAD show an efficiency of 12.8%.

关键词： Dopant-flee Perovskite solar cell Hole transport material Phenoxazine Thin fiim

基于钌络合物催化水氧化反应中的质子传递调节:不止第二配位环境

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Science Bulletin 2023年第9期68卷 854-856页

作者：刘天奇孙立成 department of chemistry School of Engineering Sciences in ChemistryBiotechnology and HealthKTH Royal Institute of TechnologyStockholm 10044Sweden centre of artificial photosynthesis for solar fuels and department of chemistry School of ScienceWestlake UniversityHangzhou 310024China

Proton transfer is a pivotal chemical process that occurs in a wide range of enzymatic *** example is the identification of several water channels near the oxygen-evolving complex in photosystem II(OEC in PSII),which ... 详细信息

关键词：质子传递钌络合物配位环境

Self-Assembled Protein Hybrid Nanofibrils for Photosynthetic Hydrogen Evolution

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CCS chemistry 2024年第3期6卷 812-823页

作者： Weijian Chen Xiantao Hu Andi Hu Luyang Ji Yiming Huang Hao Heng Fude Feng Shu Wang department of Polymer Science and Engineering School of Chemistry and Chemical EngineeringNanjing UniversityJiangsuNanjing 210023 Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190

In artificial photosynthesis systems,synthetic diiron complexes are popular[FeFe]-hydrogenase mimics,which are attractive for the fabrication of photocatalyst-protein hybrid structures to amplify hydrogen(H2)generation ***,constructing a highly bionic and efficient catalytic hybrid system is a major ***,we designed an ideal hybrid nanofibrils system that incorporates the crucial components:(1)a[FeFe]-H2ase mimic,which has a three-arm architecture(named triFeFe)for more interaction sites and higher catalytic activity and(2)uniform hybrid nanofibrils as the biological environment in which cysteine-catalyst coordination and the hydrogen-bonding network play a vital role in both catalyst binding and hydrogen evolution reaction *** assembled hybrid nanofibrils achieve efficient H2 generation with a turnover number of 2.3×103,outperforming previously reported diiron catalyst-protein hybrid ***,the hybrid nanofibrils work with photosynthetic thylakoids to produce H2,without extra photosensitizers or electron shuttle proteins,which advances the bioengineering of living systems for solar-driven biofuel production.

关键词： hybrid photocatalyst in situ assembly amyloid fibrils photosynthetic hydrogen evolution thylakoid

Tuning redox potentials of CO_2 reduction catalysts for carbon photofixation by Si nanowires

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Science China Materials 2015年第7期58卷 515-520页

作者：刘睿 Carolynn Stephani Kian L.Tan 王敦伟 Merkert chemistry Center Department of Chemistry Boston CollegeChestnut Hill MA 02467 USA Joint Center for artificial photosynthesis California Institute of Technology

Si nanowires(Si NWs) are shown to absorb visible light to reduce Ni catalysts into Ni0 compounds, enabling alkyne carboxylation reactions with CO2 as a carbon feedstock. The reduced Ni catalysts are effective in CO2 fixation through a 4-octyne carboxylation reaction. The reduction potentials of the Ni catalysts can be tuned from-1.35 to-0.51 V(vs. saturated calomel electrode) by altering the binding ligands. The results shed light on the nature of charge transfer from Si NWs to the catalyst for this new class of photocatalytic reactions. By controlling the CO2 reduction potential of the catalysts with carefully ligand designs, it will bring more opportunities and options to realize the highly selective, effective and sustainable CO2 reduction in the future.

关键词：镍催化剂 Ni 硅纳米线还原电位二氧化碳 CO2 工业气体

In-depth understanding the effect of electron-withdrawing/-donating groups on the interfacial carrier dynamics in naphthalimide-treated perovskite solar cells

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Journal of Energy chemistry 2023年第2期77卷 514-520,I0013页

作者： Tai Wu Rongjun Zhao Donglin Jia Linqin Wang Xiaoliang Zhang Licheng Sun Yong Hua Yunnan Key Laboratory for Micro/Nano Materials&Technology School of Materials and EnergyYunnan UniversityKunming 650091YunnanChina School of Materials Science and Engineering Beihang UniversityBeijing 100191China Center of artificial photosynthesis for solar fuels School of ScienceWestlake UniversityHangzhou 310024ZhejiangChina

Surface defect passivation of perovskite films through chemical interaction between specific functional groups and defects has been proven to be an effective technique for enhancing the performance and stability of perovskite solar cells(PSCs).However,an in-depth understanding of how these passivation materials affect the intrinsic nature of charge-carrier transfer kinetics in PSCs remains shielded so ***,we have designed two naphthalimide-based perovskite surface passivators having electronwithdrawing(-CF_(3),NSF)or electron-donating(-CH_(3),NSC)substituents for use in *** absorption spectroscopy(TA)measurements confirmed how the electron-withdrawing and electron-donating groups can efficiently turn the hot carriers(HCs)cooling and injection,and interface recombination in the *** found that NSC-passivated perovskite samples exhibit faster hot-carriers(HCs)injection from the perovskite layer into carrier transport layers before cooling to the crystal lattice compared with the NSF-based and control ones with the order:NSC>NSF>*** HCs injection is advantageous to minimize the charge-carriers recombination and improve PSCs *** carrier lifetime in NSCtreated device measured by nanosecond TA exhibits nearly~2 times longer than that of NSF-based device,which demonstrates the decreased charge-carrier recombination in NSC-treated *** expected,the power conversion efficiency(PCE)of the NSC-treated PSCs is improved to 23.04%compared with that of the device treated with NSF(21.81%).Our findings provide invaluable guide for developing highly efficient passivators to further boost PSCs photovoltaic performance.

关键词： Perovskite solar cell Defect Charge-carrier recombination Hot-carriers