Recent advances in heterojunction and interfacial engineering of perovskite solar cells(PSCs)have enabled great progress in developing highly efficient and stable devices.Nevertheless,the effect of halide choice on the formation mechanism,crystallography,and photoelectric properties of the low-dimensional phase still requires further detailed study.In this work,we present key insights into the significance of halide choice when designing passivation strategies comprising large organic spacer salts,clarifying the effect of anions on the formation of quasi-2D/3D heterojunctions.To demonstrate the importance of halide influences,we employ novel neo-pentylammonium halide salts with different halide anions(neoPAX,X=I,Br,or Cl).We find that regardless of halide selection,iodide-based(neoPA)2(FA)(n-1)Pbnl(3n+1)phases are formed above the perovskite substrate,while the added halide anions diffuse and passivate the perovskite bulk.In addition,we also find the halide choice has an influence on the degree of dimensionality(n).Comparing the three halides,we find that chloride-based salts exhibit superior crystallographic,enhanced carrier transport,and extraction compared to the iodide and bromide analogs.As a result,we report high power conversion efficiency in quasi-2D/3D PSCs,which are optimal when using chloride salts,reaching up to 23.35％,and improving long-term stability.

Xueping Liu;Thomas Webb;Linjie Dai;Kangyu Ji;Joel A.Smith;Rachel C.Kilbride;Mozhgan Yavari;Jinxin Bi;Aobo Ren;Yuanyuan Huang;Zhuo Wang;Yonglong Shen;Guosheng Shao;Stephen J.Sweeney;Steven Hinder;Hui Li;David G.Lidzey;Samuel D.Stranks;Neil C.Greenham;S.Ravi P.Silva;Wei Zhang

State Center for International Cooperation on Designer Low-carbon&Environmental Materials(CDLCEM),Zhengzhou University,Zhengzhou 450001,China;Advanced Technology Institute,Department of Electrical and Electronic Engineering,University of Surrey,Guildford GU2 7XH,UK;Cavendish Laboratory,University of Cambridge,Cambridge CB3 0HE,UK;Department of Physics and Astronomy,University of Sheffield,Sheffield S37RH,UK;Department of Physics,University of Oxford,Clarendon Laboratory,Oxford OX1 3PU,UK;Advanced Technology Institute and Department of Physics,University of Surrey,Guildford GU2 7XH,UK;The Surface Analysis Laboratory,Department of Mechanical Engineering Sciences,University of Surrey,Guildford GU2 7XH,UK;Institute of Electrical Engineering,Chinese Academy of Sciences,Beijing 100190,China;Department of Chemical Engineering and Biotechnology,University of Cambridge,Cambridge CB3 0AS,UK

能源与环境材料（英文）

[1]Xueping Liu;Thomas Webb;Linjie Dai;Kangyu Ji;Joel A.Smith;Rachel C.Kilbride;Mozhgan Yavari;Jinxin Bi;Aobo Ren;Yuanyuan Huang;Zhuo Wang;Yonglong Shen;Guosheng Shao;Stephen J.Sweeney;Steven Hinder;Hui Li;David G.Lidzey;Samuel D.Stranks;Neil C.Greenham;S.Ravi P.Silva;Wei Zhang-.Influence of Halide Choice on Formation of Low-Dimensional Perovskite Interlayer in Efficient Perovskite Solar Cells)[J].能源与环境材料（英文）,2022(02):670-682

pentylammonium,neoPAX,neoPA,Pbnl,3n+1

Influence,Halide,Choice,Formation,Low,Dimensional,Perovskite,Interlayer,Efficient,Solar,Cells,Recent,advances,interfacial,engineering,perovskite,solar,cells,PSCs,have,enabled,great,progress,developing,highly,efficient,stable,devices,Nevertheless,effect,choice,formation,mechanism,crystallography,photoelectric,properties,low,still,requires,further,detailed,study,this,work,present,key,insights,into,significance,when,designing,passivation,strategies,comprising,large,organic,spacer,salts,clarifying,anions,quasi,2D,heterojunctions,To,demonstrate,importance,influences,employ,novel,different,Br,Cl,We,find,that,regardless,selection,iodide,FA,phases,formed,above,substrate,while,added,diffuse,passivate,bulk,addition,also,degree,dimensionality,Comparing,three,halides,chloride,exhibit,superior,crystallographic,enhanced,carrier,transport,extraction,compared,bromide,analogs,result,report,power,conversion,efficiency,which,optimal,using,reaching,improving,long,term,stability

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