文献类型：期刊文献

英文题名：Gram-Level Production of Atomic-Scale and Photoresponsive Two-Dimensional Self-Folded Monolayer Polymeric Sheets

作者：Wu, Pengchao[1];Sui, Pengliang[1];Xu, Zejiang[1];Zheng, Yongli[2];Zhi, Dongyan[1];Zhou, Yongfeng[2];Lin, Shaoliang[1];Jin, Haibao[1]

机构：[1]East China Univ Sci & Technol, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Mat Sci & Engn, Shanghai Key Lab Adv Polymer Mat, Shanghai 200237, Peoples R China;[2]Shanghai Jiao Tong Univ, Frontiers Sci Ctr Transformat Mol, Sch Chem & Chem Engn, State Key Lab Met Matrix Composites, Shanghai 200240, Peoples R China

年份：2025

卷号：58

期号：10

起止页码：5135

外文期刊名：MACROMOLECULES

收录：;EI(收录号：20251918392289);WOS:【SCI-EXPANDED(收录号:WOS:001485227700001)】；

基金：Financial support was provided by the National Natural Science Foundation of China (52373114, 52325308, 52073092, 22231007, and 22001071). The authors thank the Research Center of Analysis and Test of East China University of Science and Technology for the help with the characterization.

语种：英文

外文关键词：Nanocomposites - Self assembly

摘要：Self-folding 1D polymers into atomic-scale and stimuli-responsive 2D polymeric nanomaterials with a scalable production and tailored functions offers an unprecedented and challenging strategy for the construction of innovative free-standing sub-1 nm 2D materials for heterogeneous catalysis. Herein, self-folded monolayer polymeric sheets (SFMPSs) with a thickness of 7.2 +/- 2.2 & Aring; and a lateral size of several hundreds of mu m2 are produced in a grams-level using the solution self-assembly of alternating azocopolymers, exemplifying the thinnest 2D self-assembled polymeric materials. A phototriggered reversible structural transformation from 2D SFMPSs to spherical micelles (SMs, similar to 32 nm) is rendered by the photoisomerization of azobenzene units. A series of SFMPS-based single-atom catalysts (SACs) is yielded using the coordination interaction between Pt ions and distinct nitrogenous ligands. The resulting photocontrollable electrocatalytic activity highly depends on the presence of the Pt element, structural characteristics of supports, and metal-support interaction. Among them, Pt-based hybrid SACs using porphyrin-modified SFMPSs as support display a favorable electrocatalytic capacity with an overpotential of similar to 22 mV at a current density of 10 mA cm-2, whose mass activity is similar to 159 times larger than commercial Pt/C catalysts. Our work proposes a significant approach to fabricating a scalable production of atomic-scale 2D macromolecular materials with controllable HER catalytic performance.