End Group-Induced Ultrafast Exciton Dissociation of Supramolecular Perylene Monoimide Nanoribbons for Efficient Photocatalytic Hydrogen Evolution - Details

author：

Indexed by：

EI

Abstract：

Achieving　fast　exciton　dissociation　is　a　critical　factor　for　optimizing　the　performance　of　organic　photocatalysts　in　solar　energy　conversion.　This　work　demonstrates　the　end-group-dependent　ultrafast　exciton　dissociation　in　supramolecular　perylene　monoimide　(PMI)　nanostructures.　A　series　of　PMI　molecules　are　designed　by　connecting　the　amide　site　with　methylene　carboxyl　(─CH2─COOH),　methylene　phosphonic　acid　(─CH2─PO3H2),　and　methylene　sulfonic　acid　(─CH2─SO3H)　to　increase　the　dipole　moment　and　built-in　electric　field,　thereby　effectively　diminishing　exciton　binding　energy.　Upon　photoexcitation,　self-assembled　PMI-CH2-SO3H　nanoribbons　(NRs),　which　exhibit　the　lowest　exciton　binding　energy　of　29.4　meV,　achieve　ultrafast　exciton　dissociation　within　0.25 ps,　leading　to　the　formation　of　charge-separated　excitons　from　charge-transfer　states.　This　dissociation　rate　is　≈40　and　16　times　faster　than　that　observed　in　PMI-CH2-COOH　(NRs)　and　PMI-CH2-PO3H2　(NRs),　respectively.　Following　the　deposition　of　Pt　nanoparticles　on　PMI　NRs,　Pt/PMI-CH2-SO3H　(NRs)　demonstrates　an　H2　evolution　of　21.2　mmol　g−1　h−1　under　visible　light　irradiation　(λ　＞ 420 nm),　outperforming　Pt/PMI-CH2-COOH　(NRs)　and　Pt/PMI-CH2-PO3H2　(NRs)　by　factors　of　53　and　5.4,　respectively.　©　2025　Wiley-VCH　GmbH.

Keyword：

Carrier concentration Excitons Nanoribbons Photocatalysis Photoexcitation Solar power generation Surface discharges

Community：

[ 1 ] [Wu, Shuhong]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350108, China
[ 2 ] [Cheng, Xiuyan]Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou; 350002, China
[ 3 ] [Huang, Haowei]School of Energy and Environment, Southeast University, Nanjing; 210096, China
[ 4 ] [Yang, Qin]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350108, China
[ 5 ] [Wang, Ying]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350108, China
[ 6 ] [Zhuang, Yan]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350108, China
[ 7 ] [Li, Wanqing]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350108, China
[ 8 ] [Liu, Yuan]State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian; 110623, China
[ 9 ] [Lin, Huan]Beijing Key Laboratory for Green Catalysis and Separation, College of Materials Science and Engineering, Beijing University of Technology, Beijing; 100124, China
[ 10 ] [Niu, Hui]Beijing Key Laboratory for Green Catalysis and Separation, College of Materials Science and Engineering, Beijing University of Technology, Beijing; 100124, China
[ 11 ] [Wang, Junhui]State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian; 110623, China
[ 12 ] [Wu, Kaifeng]State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian; 110623, China
[ 13 ] [Fu, Xianzhi]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350108, China
[ 14 ] [Long, Jinlin]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350108, China

Reprint 's Address：

[huang, haowei]school of energy and environment, southeast university, nanjing; 210096, china

Email：

jllong@fzu.edu.cnhaowei.huang@seu.edu.cn

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