近日，大连理工大学郭新闻及其小组通过提高聚七嗪亚胺（PHI）纳米棒远程有序度的自下而上策略，实现了高效光催化CO₂甲烷化。该研究于2024年12月3日发表于国际一流学术期刊《德国应用化学》。

研究人员表示，聚七嗪亚胺（PHI）是一种极具发展前景的聚合物光催化剂，是聚合物氮化碳的晶体或远程有序同素异形体之一。然而，制备高结晶PHI仍然是一个挑战。

该研究采用自下向上方法，包括修复结构缺陷，增加瓜前驱体的比表面积，制备了远端有序度显著提高的PHI纳米棒。与具有较低长程序的原始PHI相比下，由此产生的PHI在CO₂光还原过程中表现出从CO到CH₄的产物选择性转变，具有较高的甲烷化活性。

PHI长程序的改善显著提高了光生电荷的分离效率、传递动力学以及对*CO中间体的吸附能力。该研究揭示了离子热合成过程中前驱体结构与PHI晶体生长之间的关系，也展示了高结晶PHI在人工光合作用中的巨大潜力。

附：英文原文

Title: Bottom-Up Strategy to Enhance Long-Range Order of Poly(Heptazine Imide) Nanorods for Efficient Photocatalytic CO2 Methanation

Author: Jiaming Wu, Keyan Li, Bing Zhou, Rui Li, Siyang Yan, Jiaxu Liu, Hainan Shi, Chunshan Song, Xinwen Guo

Issue&Volume: 2024-12-03

Abstract: Poly(heptazine imide) (PHI), one of the crystalline or long-range ordered allotropes of polymeric carbon nitride, is a promising polymeric photocatalyst; however, preparation of highly crystalline PHI remains a challenge. Herein, through a bottom-up strategy involving repair of structural defects and increase of specific surface area of melon precursor, we prepared PHI nanorods with dramatically improved long-range order. The resulting PHI exhibited a shift of product selectivity in CO2 photoreduction from CO to CH4 with a high methanation activity in contrast to the pristine PHI with relatively low long-range order. The improvement of long-range order for PHI remarkably enhanced the separation efficiency and transfer dynamics of photogenerated charges as well as the adsorption capacity for *CO intermediate. This study revealed the relationship between the precursor structure and PHI crystal growth in ionothermal synthesis, and also showcased the great potential of highly crystalline PHI in artificial photosynthesis.

DOI: 10.1002/anie.202421263

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202421263