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Polymeric viologen-based electron transfer mediator for improving the photoelectrochemical water splitting on Sb_(2)Se_(3) photocathode

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Fundamental Research 2024年第2期4卷 291-299页

作者： Chang Liu Fusheng Li Linqin Wang Zeju Li Yilong Zhao Yingzheng Li Wenlong Li Ziqi Zhao Ke Fan Fei Li Licheng Sun State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT-KTH Joint Education and Research Centre on Molecular DevicesInstitute for Energy Science and TechnologyDalian University of TechnologyDalian 116024China Center of artificial photosynthesis for solar fuels School of ScienceWestlake UniversityHangzhou 310024China department of chemistry School of Engineering Sciences in ChemistryBiotechnology and HealthKTH Royal Institute of TechnologyStockholm 10044Sweden

The photogenerated charge carrier separation and transportation of inside photocathodes can greatly influence the performance of photoelectrochemical(PEC)H2 production devices.Coupling TiO_(2) with p-type semiconductors to construct heterojunction structures is one of the most widely used strategies to facilitate charge separation and transportation.However,the band position of TiO_(2) could not perfectly match with all p-type semiconductors.Here,taking antimony selenide(Sb_(2)Se_(3))as an example,a rational strategy was developed by introducing a viologen electron transfer mediator(ETM)containing polymeric film(poly-1,1′-dially-[4,4′-bipyridine]-1,1′-diium,denoted as PV^(2+))at the interface between Sb_(2)Se_(3) and TiO_(2) to regulate the energy band alignment,which could inhibit the recombination of photogenerated charge carriers of interfaces.With Pt as a catalyst,the constructed Sb_(2)Se_(3)/PV^(2+)/TiO_(2)/Pt photocathode showed a superior PEC hydrogen generation activity with a photocurrent density of−18.6 mA cm^(-2) vs.a reversible hydrogen electrode(RHE)and a half-cell solar-to-hydrogen efficiency(HC-STH)of 1.54%at 0.17 V vs.RHE,which was much better than that of the related Sb_(2)Se_(3)/TiO_(2)/Pt photocathode without PV^(2+)(−9.8 mA cm^(-2),0.51%at 0.10 V vs.RHE).

关键词： Viologen Electron transfer mediator Sb2Se3 photocathode solar water splitting Hydrogen evolution reaction

Influence of O-O formation pathways and charge transfer mediator on lipid bilayer membrane-like photoanodes for water oxidation

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Journal of Energy chemistry 2024年第6期93卷 526-537,I0013页

作者： Yingzheng Li Shaoqi Zhan Zijian Deng Meng Chen Yilong Zhao Chang Liu Ziqi Zhao Hongxia Ning Wenlong Li Fei Li Licheng Sun Fusheng Li State Key Laboratory of Fine Chemicals Frontier Science Center for Smart MaterialsDalian University of Technology116024 DalianLiaoningChina department of chemistry-Ångström Uppsala UniversityBox 52375120 Uppsal1Sweden Center of artificial photosynthesis for solar fuels School of ScienceWestlake UniversityHangzhou 310024ZhejiangChina

Inspired by the function of crucial components in photosystemⅡ(PSⅡ),electrochemical and dyesensitized photoelectrochemical(DSPEC)water oxidation devices were constructed by the selfassembly of well-designed amphipathic Ru(bda)-based catalysts(bda=2,2'-bipyrdine-6,6'-dicarbonoxyl acid)and aliphatic chain decorated electrode surfaces,forming lipid bilayer membrane(LBM)-like structures.The Ru(bda)catalysts on electrode-supported LBM films demonstrated remarkable water oxidation performance with different O-O formation mechanisms.However,compared to the slow charge transfer process,the O-O formation pathways did not determine the PEC water oxidation efficiency of the dyesensitized photoanodes,and the different reaction rates for similar catalysts with different catalytic paths did not determine the PEC performance of the DSPECs.Instead,charge transfer plays a decisive role in the PEC water oxidation rate.When an indolo[3,2-b]carbazole derivative was introduced between the Ru(bda)catalysts and aliphatic chain-modified photosensitizer in LBM films,serving as a charge transfer mediator for the tyrosine-histidine pair in PSⅡ,the PEC water oxidation performance of the corresponding photoanodes was dramatically enhanced.

关键词： Water oxidation Rate determine step Dye-sensitized photoelectrochemical cell Charge transfer artificial photosynthesis

Precursor engineering enables high-performance all-inorganic CsPbIBr_(2) perovskite solar cells with a record efficiency approaching 13%

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Journal of Energy chemistry 2024年第3期90卷 16-22,I0003页

作者： Qingyan Chang Yidan An Huaiman Cao Yuzhen Pan Liangyu Zhao Yulong Chen Yi We Sai-Wing Tsang Hin-Lap Yip Licheng Sun Ze Yu State Key Laboratory of Fine Chemicals Dalian University of Technology(DUT)Dalian 116024LiaoningChina department of Materials Science and Engineering City University of Hong KongKowloon 999077Hong KongChina School of chemistry Dalian University of Technology(DUT)Dalian 116024LiaoningChina Key Laboratory of Materials Modification by Laser Ionand Electron Beams(Ministry of Education)Dalian University of Technology(DUT)Dalian 116024LiaoningChina School of Energy and Environment City University of Hong KongKowloon 999077Hong KongChina Center of artificial photosynthesis for solar fuels and department of chemistry School of ScienceWestlake UniversityHangzhou 310024ZhejiangChina department of chemistry School of Engineering Sciences in ChemistryBiotechnology and HealthKTH Royal Institute of Technology10044 StockholmSweden

All-inorganic CsPbIBr_(2) perovskite has attracted widespread attention in photovoltaic and other optoelectronic devices because of its superior thermal stability.However,the deposition of high-quality solutionprocessed CsPbIBr_(2) perovskite films with large thicknesses remains challenging.Here,we develop a triple-component precursor(TCP) by employing lead bromide,lead iodide,and cesium bromide,to replace the most commonly used double-component precursor(DCP) consisting of lead bromide and cesium iodide.Remarkably,the TCP system significantly increases the solution concentration to 1.3 M,leading to a larger film thickness(~390 nm) and enhanced light absorption.The resultant CsPbIBr_(2) films were evaluated in planar n-i-p structured solar cells,which exhibit a considerably higher optimal photocurrent density of 11.50 mA cm^(-2) in comparison to that of DCP-based devices(10.69 mA cm^(-2)).By adopting an organic surface passivator,the maximum device efficiency using TCP is further boosted to a record efficiency of 12.8% for CsPbIBr_(2) perovskite solar cells.

关键词： All-inorganic perovskite solar cells CsPbIBr_(2) Precursor engineering Solubility High performance

Copper naphthalocyanine-based hole-transport material for highperformance and thermally stable perovskite solar cells

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Science China chemistry 2024年第8期67卷 2701-2709页

作者： Yue Qiang Huaiman Cao Yuzhen Pan Yi Chi Liangyu Zhao Yingguo Yang Hai-Bei Li Yan Gao Licheng Sun Ze Yu State Key Laboratory of Fine Chemicals Frontier Science Center for Smart Materials Dalian University of Technology (DUT) School of chemistry Dalian University of Technology (DUT) School of Microelectronics Fudan University Shanghai Synchrotron Radiation Facility (SSRF) Zhangjiang Lab Shanghai Advanced Research InstituteShanghai Institute of Applied Physics Chinese Academy of Sciences School of Ocean Shandong University Center of artificial photosynthesis for solar fuels and department of chemistry School of Science Westlake University department of chemistry School of Engineering Sciences in Chemistry Biotechnology and Health KTH Royal Institute of Technology

Metal phthalocyanines（MPcs） have gained considerable research attention as hole-transport materials（HTMs） in perovskite solar cells（PSCs） because of their superb stability. However, the photovoltaic performance of MPc-based HTMs in PSCs is still lagging behind their small molecule and polymeric counterparts, largely due to their relatively low hole mobility. Here, we report for the first time the application of a copper naphthalocyanine derivative（namely t Bu-Cu Nc） as a hole-transport material（HTM）in perovskite solar cells（PSCs）, and systematically study its optoelectronic and photovoltaic property compared with its Cu Pc analog（t Bu-Cu Pc）. Combined experiments disclose that the extension of π-conjugation from Pc to Nc core leads to not only an enhanced hole-carrier mobility associated with a stronger intermolecular interaction, but also an elevated glass transition temperature（Tg） of 252 °C. The resultant PSCs employing t Bu-Cu Nc deliver an excellent power conversion efficiency of 24.03%, which is the record efficiency reported for metal complex-based HTMs in PSCs. More importantly, the encapsulated t Bu-Cu Nc-based devices also show dramatically improved thermal stability than the devices using the well-known SpiroOMe TAD, with a T80lifetime for more than 1,000 h under damp-heat stress. This study unfolds a new avenue for developing efficient and stable HTMs in PSCs.

关键词：

Improving performance of Cs_(2)AgBiBr_(6)solar cell through constructing gradient energy level with deep-level hole transport material

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稀有金属:英文版 2023年第9期42卷 3004-3012页

作者： Zi-Yang Xia Wei Zhang Cheng Chen Hao-Xin Wang Lin-Qin Wang Ya-Wei Miao Xing-Dong Ding Li-Cheng Sun Ming Cheng Institute for Energy Research School of Energy and Power EngineeringJiangsu UniversityZhenjiang212013China Center of artificial photosynthesis for solar fuels and department of chemistry School of ScienceWestlake UniversityHangzhou310024China

The valence band offset between Cs_(2)AgBiBr_(6)and hole transport layer(HTL)is approximately 1.00 e V,which results in high energy loss and is identified as one of the bottle necks of Cs_(2)Ag BiBr_(6)perovskite solar cell(PSC)for achieving high power conversion efficiency(PCE).To tackle this problem,we propose the optimization of the energy level alignment by designing and synthesizing novel deep-level hole transport materials(HTMs).The sole introduction of deep-level HTMs successfully reduces the valence band offset between Cs_(2)Ag Bi Br_(6)and HTL,but induces the increased valence band offset at HTL/Au interface,limiting the PCE improvement.To further solve the problem and improve the PCE,the gradient energy level arrangement is constructed by combining the newly developed deep-level HTM 6,6’-(3-((9,9-dimethyl-9H-fluoren-3-yl)(4-methoxyphenyl)amino)thiophene-2,5-diyl)bis(N-(9,9-dimethyl-9H-fluoren-2-yl)-N,9-bis(4-methoxyphenyl)-9H-carbazol-3-amine)(TF)with 2,2’,7,7’-tetrakis(N,N’-dipmethoxyphenylamine)-9,9-spirobifluorene(Spiro-OMeTAD).Through optimization,an impressive PCE of 3.50%with remarkably high open-circuit voltage(V_(oc))and fill factor(FF)is achieved,qualifying it among the best pristine Cs_(2)AgBiBr_(6)PSCs.

关键词： All-inorganic Cs_(2)AgBiBr_(6)perovskite Stepped energy level structure Energy loss Moisture resistance

Promotion of the oxygen evolution performance of Ni–Fe layered hydroxides via the introduction of a proton-transfer mediator anion

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Science China chemistry 2022年第2期65卷 382-390页

作者： Wenlong Li Fusheng Li Yilong Zhao Chang Liu Yingzheng Li Hao Yang Ke Fan Peili Zhang Yu Shan Licheng Sun State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT-KTH Joint Education and Research Centre on Molecular DevicesDalian University of TechnologyDalian 116024China 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 310024China

Developing efficient catalysts with high durability and activity for the oxygen evolution reaction(OER)is imperative for sustainable energy conversion technologies,including hydrogen generation and CO_(2) reduction,as well as other electrochemical energy storage systems.To this end,a comprehensive understanding of the mechanism for the water oxidation reaction is vital.Herein,a surfactant,nonafluoro-1-butanesulfonate(FBS),was introduced into Ni-Fe layered double hydroxide(Ni Fe-FBS/CFP)via electrochemical deposition on the surface of a carbon fiber paper(CFP)substrate.The as-prepared Ni Fe-FBS/CFP electrode exhibited excellent catalytic activities for OER compared to the Ni-Fe layered double hydroxide based electrode(Ni Fe-LDH/CFP),an excellent stability of 15 h,and an ultralow Tafel slope of 25.8 m V dec-1.Furthermore,by combining the results of p H-dependent kinetics investigations,chemical probing,proton inventory studies,and isotopic and atom-protontransfer measurements,it was observed that a proton-transfer process controls the reaction rates of both the Ni Fe-LDH and Ni Fe-FBS catalysts,and the residual sulfonate groups serve as proton transfer mediator to accelerate the proton transfer rate.

关键词： water splitting Ni Fe–LDH proton-coupled electron transfer proton transfer mediator sulfonate group

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 urgently.photosynthesis in nature converts CO2and H2O into carbohydrates and O2and is driven by solar energy via photosystemⅡ(PSⅡ) and photosystemⅠ(PSI)[1].Water oxidation occurring at the oxygen-evolution complex (OEC:

关键词：

The future challenges in molecular water oxidation catalysts

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Journal of Energy chemistry 2022年第10期31卷 643-645,I0016页

作者： Tianqi Liu Licheng Sun department of chemistry School of Engineering Sciences in Chemistry Biotechnology and HealthKTH Royal Institute of Technology10044 StockholmSweden State Key Laboratory of Fine Chemicals Dalian University of Technology(DUT)Dalian 116024LiaoningChina centre of artificial photosynthesis for solar fuels and department of chemistry School of ScienceWestlake UniversityHangzhou 310024ZhejiangChina

Energy is the bedrock of a functioning society,and artificial photosynthesis provides a possible solution for the generation of clean and affordable energy by storing the power of sunlight in chemical fuels via proton... 详细信息

关键词： dioxide afford artificial

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 reactions.One example is the identification of several water channels near the oxygen-evolving complex in photosystem II(OEC in PS... 详细信息

关键词：质子传递钌络合物配位环境