학술논문
基于溶液化学策略构建背接触FTO/赤铁矿光阳极界面工程的高效光催化水氧化 / Solution chemistry back-contact FTO/hematite interface engineering for efficient photocatalytic water oxidation
Document Type
Academic Journal
Author
Source
催化学报 / Chinese Journal of Catalysis. 43(5):1247-1257
Subject
Language
Chinese
ISSN
0253-9837
Abstract
本文采用一种简单、有效的规模化溶液化学策略,在基底(如商用氟掺杂氧化锡透明导电涂层玻璃(FTO))和光活性薄膜(如赤铁矿)之间形成丰富的背接触界面,并用于低成本水氧化反应.高分辨率电子显微镜(扫描电镜、透射电镜、扫描透射电镜)、原子力显微镜、元素成像(电子能量损失谱和能量色散谱)和光电化学研究表明,可通过前驱体溶液的化学成分工程来有效降低机械应力、晶格失配、电子势垒和FTO与赤铁矿在背面接触界面之间的空隙以及FTO与电解液之间的短路和有害反应,进而提升这些低成本光阳极对水氧化反应以及PEC水分解清洁、可持续地生产氢气的整体效率.本研究对通过最小化在介孔电极的背接触界面和晶粒边界上的电子-空穴复合,进而提高电荷收集效率具有重要意义,可提高低成本PEC水裂解装置的整体效率和规模化的能力.
This work describes a simple yet powerful scalable solution chemistry strategy to create back-contact rich interfaces between substrates such as commercial transparent conducting fluo-rine-doped tin oxide coated glass (FTO) and photoactive thin films such as hematite for low-cost water oxidation reaction. High-resolution electron microscopy (SEM, TEM, STEM), atomic force microscopy (AFM), elemental chemical mapping (EELS, EDS) and photoelectrochemical (PEC) in-vestigations reveal that the mechanical stress, lattice mismatch, electron energy barrier, and voids between FTO and hematite at the back-contact interface as well as short-circuit and detrimental reaction between FTO and the electrolyte can be alleviated by engineering the chemical composi-tion of the precursor solutions, thus increasing the overall efficiency of these low-cost photoanodes for water oxidation reaction for a clean and sustainable generation of hydrogen from PEC wa-ter-splitting. These findings are of significant importance to improve the charge collection efficiency by minimizing electron-hole recombination observed at back-contact interfaces and grain bounda-ries in mesoporous electrodes, thus improving the overall efficiency and scalability of low-cost PEC water splitting devices.
This work describes a simple yet powerful scalable solution chemistry strategy to create back-contact rich interfaces between substrates such as commercial transparent conducting fluo-rine-doped tin oxide coated glass (FTO) and photoactive thin films such as hematite for low-cost water oxidation reaction. High-resolution electron microscopy (SEM, TEM, STEM), atomic force microscopy (AFM), elemental chemical mapping (EELS, EDS) and photoelectrochemical (PEC) in-vestigations reveal that the mechanical stress, lattice mismatch, electron energy barrier, and voids between FTO and hematite at the back-contact interface as well as short-circuit and detrimental reaction between FTO and the electrolyte can be alleviated by engineering the chemical composi-tion of the precursor solutions, thus increasing the overall efficiency of these low-cost photoanodes for water oxidation reaction for a clean and sustainable generation of hydrogen from PEC wa-ter-splitting. These findings are of significant importance to improve the charge collection efficiency by minimizing electron-hole recombination observed at back-contact interfaces and grain bounda-ries in mesoporous electrodes, thus improving the overall efficiency and scalability of low-cost PEC water splitting devices.