Replication data of Lotsch group for: "Covalent Organic Framework Nanoplates Enable Solution-Processed Crystalline Nanofilms for Photoelectrochemical Hydrogen Evolution"

As covalent organic frameworks (COFs) are coming of age, the lack of effective approaches to achieve crystalline and centimeter-scale-homogeneous COF films remains a significant bottleneck toward advancing the application of COFs in optoelectronic devices. Here, we present the synthesis of colloidal COF nanoplates, with lateral sizes of ∼200 nm and average heights of 35 nm, and their utilization as photocathodes for solar hydrogen evolution. The resulting COF nanoplate colloid exhibits a unimodal particle-size distribution and an exceptional colloidal stability without showing agglomeration after storage for 10 months and enables smooth, homogeneous, and thickness-tunable COF nanofilms via spin coating. Photoelectrodes comprising COF nanofilms were fabricated for photoelectrochemical (PEC) solar-to-hydrogen conversion. By rationally designing multicomponent photoelectrode architectures including a polymer donor/COF heterojunction and a hole-transport layer, charge recombination in COFs is mitigated, resulting in a significantly increased photocurrent density and an extremely positive onset potential for PEC hydrogen evolution (over +1 V against the reversible hydrogen electrode), among the best of classical semiconductor-based photocathodes. This work thus paves the way toward fabricating solution-processed large-scale COF nanofilms and heterojunction architectures and their use in solar-energy-conversion devices. All primary data files of measurements and processed data of the journal article mentioned under related publications from Lotsch group can be found here. The data is structured according to figures and schemes in the research article and contains the following data types: XRD patterns (*.raw), AFM images (*.ibw), Nitrogen isotherm profiles (*.qps), dynamic light scattering data (*.dts), TEM images (*.dm3), ChemDraw files (*.cdxml), NMR data (*.jdf, *.mnova), python jupyter files (*.ipynb), CorelDraw files (*.cdr), SEM images (*.tif), electrochemistry data (*.paax), origin files (*.opju), COF structure models (*.cif), and FT-IR spectra (*.sp).

随着共价有机框架（COFs）技术的成熟，实现晶体化和厘米级均质COF薄膜的有效方法仍然是其应用于光电设备领域的一个重大瓶颈。本研究中，我们展示了具有横向尺寸约为200纳米和平均高度为35纳米的胶体COF纳米片的合成，并将其作为光阴极应用于太阳能制氢。所得到的COF纳米片胶体表现出单峰的粒径分布和卓越的胶体稳定性，在储存10个月后未见团聚现象，并通过旋涂技术实现了平滑、均匀且厚度可调的COF纳米薄膜。由COF纳米薄膜构成的电极被用于光化学（PEC）太阳能转化为氢能。通过合理设计多组分光电极结构，包括聚合物供体/COF异质结和空穴传输层，有效降低了COFs中的电荷复合，从而显著提高了光电流密度和光化学氢析出（相对于可逆氢电极，超过+1伏）的起始电位，在经典半导体基光电阴极中表现优异。因此，本研究为制造溶液处理的规模化COF纳米薄膜和异质结结构及其在太阳能转换设备中的应用铺平了道路。相关出版物中提及的Lotz小组所发表的期刊文章的所有原始测量数据和处理数据文件均可在本处找到。数据结构遵循研究文章中的图和方案，并包含以下数据类型：XRD图谱 (*.raw)，原子力显微镜图像 (*.ibw)，氮气等温线图谱 (*.qps)，动态光散射数据 (*.dts)，透射电子显微镜图像 (*.dm3)，ChemDraw文件 (*.cdxml)，核磁共振数据 (*.jdf, *.mnova)，Python Jupyter文件 (*.ipynb)，CorelDraw文件 (*.cdr)，扫描电子显微镜图像 (*.tif)，电化学数据 (*.paax)，Origin文件 (*.opju)，COF结构模型 (*.cif)，和傅里叶变换红外光谱 (*.sp)。