Yang Lin, Zheng Tianfang, Liu Ziyan, Shibayama Naoyuki, Li Peng, Ma Jiangang, Zhang Xintong, Zhu Hancheng, Wang Xiao-Feng, Xu Haiyang, Liu Yichun
State Key Laboratory of Integrated Optoelectronics, Key Laboratory for UV-Emitting Materials and Technology of Ministry of Education, School of Physics, Northeast Normal University, 5268 Renmin Street, Changchun, 130024, China.
Key Laboratory of Physics and Technology for Advanced Batteries (Ministry of Education), College of Physics, Jilin University, Changchun, 130012, China.
Adv Sci (Weinh). 2025 Sep;12(33):e06567. doi: 10.1002/advs.202506567. Epub 2025 Jun 29.
MXenes have demonstrated exceptional performance in energy applications, yet their potential in photovoltaic systems, particularly in lead-free perovskite solar cells (PSCs), remains underexplored, with no strategic studies addressing how MXene composition influences critical photovoltaic performance. Here, we present the first strategic screening of MX-type MXenes (including HfCT, ZrCT, TaCT, NbCT, MoCT, and VCT) for rational heterojunction design with CsAgBiBr, focusing on the interplay between properties of MXenes and photovoltaic performance. Density functional theory (DFT) calculations reveal that MXenes can induce substantial electronic states near the Fermi level, creating superior charge transfer paths in CsAgBiBr, with VCT exhibiting the lowest interfacial contact barrier and the highest carrier transfer efficiency. Complementary ab initio molecular dynamics (AIMD) simulations coupled with X-ray photoelectron spectroscopy analyses further demonstrate that the functional termination groups like ─F in MXenes effectively passivate Br vacancies in CsAgBiBr, thereby enhancing crystallization and suppressing defect densities. Consequently, the experimental results yielded a trend in line with the calculations, and the power conversion efficiency (PCE) of the device with VCT represented a 36% improvement, accompanied by exceptional stability. By establishing quantitative structure-property relationships between MXenes and CsAgBiBr, this work provides a universal materials selection paradigm for developing high-performance, environmentally-friendly photovoltaic technologies.
MXenes在能源应用中已展现出卓越性能，然而它们在光伏系统中的潜力，尤其是在无铅钙钛矿太阳能电池（PSCs）中的潜力，仍未得到充分探索，目前尚无针对MXene组成如何影响关键光伏性能的战略性研究。在此，我们首次对MX型MXenes（包括HfCT、ZrCT、TaCT、NbCT、MoCT和VCT）进行战略性筛选，以实现与CsAgBiBr的合理异质结设计，重点关注MXenes的性质与光伏性能之间的相互作用。密度泛函理论（DFT）计算表明，MXenes可在费米能级附近诱导大量电子态，在CsAgBiBr中创造出优异的电荷转移路径，其中VCT表现出最低的界面接触势垒和最高的载流子转移效率。互补的从头算分子动力学（AIMD）模拟与X射线光电子能谱分析进一步表明，MXenes中的─F等功能性端基可有效钝化CsAgBiBr中的Br空位，从而促进结晶并抑制缺陷密度。因此，实验结果与计算结果相符，含VCT的器件的功率转换效率（PCE）提高了36%，同时具有出色的稳定性。通过建立MXenes与CsAgBiBr之间的定量结构-性能关系，这项工作为开发高性能、环境友好型光伏技术提供了一种通用的材料选择范例。
