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Title: Two-Dimensional Polycyclic Photovoltaic Molecule with Low Trap Density for High-Performance Photocatalytic Hydrogen Evolution

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [1];  [2];  [3];  [1];  [2]; ORCiD logo [1]
  1. Chinese Academy of Sciences (CAS), Beijing (China); University of Chinese Academy of Sciences, Beijing (China)
  2. Xi'an Jiaotong University, Shaanxi (China)
  3. Chinese Academy of Sciences (CAS), Beijing (China)

Typical organic semiconductors show a high trap density of states (1016–1018 cm-3), providing a large number of centers for charge-carrier recombination, thus hindering the development of photocatalytic hydrogen evolution. In this report we design and synthesize a two-dimensional polycyclic photovoltaic material, named as TPP, to reduce the trap density to as low as 2.3×1015 cm-3, which is 1–3 orders of magnitude lower than those of typical organic semiconductors. Moreover, TPP exhibits a broad and strong absorption, ordered molecular packing with a large crystalline coherence length and enhanced electron mobility. Then, the bulk heterojunction nanoparticles (BHJ-NPs) based on a blend of polymer donor (PM6) and TPP exhibit an average hydrogen evolution rate (HER) of 64.31 mmol h-1 g-1 under AM1.5G sunlight (100,mW cm-2), and 72.75 mmol h-1 g-1 under 330–1100 nm illumination (198 mW cm-2) higher than that of the control NPs based on typical PM6 : Y6 (62.67 mmol h-1 g-1).

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); University of Chinese Academy of Sciences, Beijing (China)
Sponsoring Organization:
China Postdoctoral Science Foundation; Key Scientific and Technological Innovation Team Project of Shaanxi Province; National Natural Science Foundation of China; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1981386
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 10 Vol. 61; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (49)

Heterojunction Photocatalysts journal February 2017
Implementing Metal-to-Ligand Charge Transfer in Organic Semiconductor for Improved Visible-Near-Infrared Photocatalysis journal May 2016
An Electron Acceptor Analogue for Lowering Trap Density in Organic Solar Cells journal March 2021
The Effect of Residual Palladium Catalyst Contamination on the Photocatalytic Hydrogen Evolution Activity of Conjugated Polymers journal October 2018
Small Number of Defects per Nanostructure Leads to “Digital” Quenching of Photoluminescence: The Case of Metal Halide Perovskites journal October 2020
Photocatalysts Based on Organic Semiconductors with Tunable Energy Levels for Solar Fuel Applications journal September 2020
Organic Polymer Dots as Photocatalysts for Visible Light-Driven Hydrogen Generation journal September 2016
Konjugierte Polymere: Katalysatoren für die photokatalytische Wasserstoffentwicklung journal November 2016
A Rapid Microwave-Assisted Thermolysis Route to Highly Crystalline Carbon Nitrides for Efficient Hydrogen Generation journal October 2016
Organic Polymer Dots as Photocatalysts for Visible Light-Driven Hydrogen Generation journal September 2016
Conjugated Polymers: Catalysts for Photocatalytic Hydrogen Evolution journal November 2016
A Rapid Microwave‐Assisted Thermolysis Route to Highly Crystalline Carbon Nitrides for Efficient Hydrogen Generation journal October 2016
Revisiting the Limiting Factors for Overall Water‐Splitting on Organic Photocatalysts journal July 2020
TiO2@PbTiO3 core-shell nanoparticles as mesoporous layer to improve electron transport performance in carbon-based perovskite solar cells journal November 2020
Recent advances in molecular design of functional conjugated polymers for high-performance polymer solar cells journal December 2019
Soft Photocatalysis: Organic Polymers for Solar Fuel Production journal July 2016
Recent Advances in Electrocatalytic Hydrogen Evolution Using Nanoparticles journal October 2019
Design Proposals for Organic Materials Exhibiting a Low Exciton Binding Energy journal September 2015
Exciton Binding Energies of Nonfullerene Small Molecule Acceptors: Implication for Exciton Dissociation Driving Forces in Organic Solar Cells journal September 2018
Enhanced Driving Force and Charge Separation Efficiency of Protonated g-C 3 N 4 for Photocatalytic O 2 Evolution journal October 2015
Selenium Heterocyclic Electron Acceptor with Small Urbach Energy for As-Cast High-Performance Organic Solar Cells journal October 2020
Panchromatic Ternary Polymer Dots Involving Sub-Picosecond Energy and Charge Transfer for Efficient and Stable Photocatalytic Hydrogen Evolution journal February 2021
Asymmetric Glycolated Substitution for Enhanced Permittivity and Ecocompatibility of High-Performance Photovoltaic Electron Acceptor journal August 2021
H- and J-Aggregation of Fluorene-Based Chromophores journal December 2014
Electrochemical Photolysis of Water at a Semiconductor Electrode journal July 1972
Particulate photocatalysts for overall water splitting journal August 2017
Determining the optimum morphology in high-performance polymer-fullerene organic photovoltaic cells journal December 2013
Photocatalytic hydrogen generation from hydriodic acid using methylammonium lead iodide in dynamic equilibrium with aqueous solution journal December 2016
Band alignment of rutile and anatase TiO2 journal July 2013
Delocalization of exciton and electron wavefunction in non-fullerene acceptor molecules enables efficient organic solar cells journal August 2020
Enhanced photocatalytic hydrogen evolution from organic semiconductor heterojunction nanoparticles journal February 2020
Intrinsic efficiency limits in low-bandgap non-fullerene acceptor organic solar cells journal October 2020
Reaction systems for solar hydrogen production via water splitting with particulate semiconductor photocatalysts journal March 2019
Earth-abundant hydrogen evolution electrocatalysts journal January 2014
A hydrazone-based covalent organic framework for photocatalytic hydrogen production journal January 2014
Exciton diffusion in organic semiconductors journal January 2015
Evolving molecular architectures of donor–acceptor conjugated polymers for photovoltaic applications: from one-dimensional to branched to two-dimensional structures journal January 2017
Characterization of semiconductor photocatalysts journal January 2019
Metal-free photocatalysts for hydrogen evolution journal January 2020
Quad-rotor-shaped non-fullerene electron acceptor materials with potential to enhance the photoelectric performance of organic solar cells journal January 2019
Charge carrier traps in organic semiconductors: a review on the underlying physics and impact on electronic devices journal January 2020
Conjugated polymer donor–molecular acceptor nanohybrids for photocatalytic hydrogen evolution journal January 2020
Development of metal-free layered semiconductors for 2D organic field-effect transistors journal January 2021
The identification, characterization and mitigation of defect states in organic photovoltaic devices: a review and outlook journal January 2013
Synthesis, optical properties and charge transport characteristics of a series of novel thiophene-fused phenazine derivatives journal January 2013
Quantitative Analysis of the Density of Trap States in Semiconductors by Electrical Transport Measurements on Low-Voltage Field-Effect Transistors journal October 2018
Trap density of states in small-molecule organic semiconductors: A quantitative comparison of thin-film transistors with single crystals journal April 2010
Scherrer grain-size analysis adapted to grazing-incidence scattering with area detectors. Erratum journal January 2013
Interface structure between titania and perovskite materials observed by quartz crystal microbalance system journal January 2015