PMID- 34405676 OWN - NLM STAT- PubMed-not-MEDLINE LR - 20210902 IS - 1944-8252 (Electronic) IS - 1944-8244 (Linking) VI - 13 IP - 34 DP - 2021 Sep 1 TI - Stiffening the Pb-X Framework through a pi-Conjugated Small-Molecule Cross-Linker for High-Performance Inorganic CsPbI(2)Br Perovskite Solar Cells. PG - 40489-40501 LID - 10.1021/acsami.1c06533 [doi] AB - Inorganic CsPbI(2)Br perovskites have witnessed incredible advances as a promising representative for translucent and tandem solar cells, but unfortunately, they are still plagued by serious energy losses and undesired phase instability. Herein, a new type of pi-conjugated small molecule of 4-guanidinobenzoic-acid-hydrochloride (4-GBACl) is demonstrated to effectively cross-link the Pb-X framework of perovskites. The strong coordination between 4-GBACl and the [PbX(6)](4-) octahedron of perovskites effectively stiffens the Pb-X framework to suppress the ion migration, thus stabilizing the perovskite phase structure against light and thermal conditions. Apart from the physical barrier for phase instability resulting from the hydrophobic benzene ring at grain boundaries (GBs), guanidinium cations and -COOH and Cl(-) groups can simultaneously afford the passivation of positively and negatively charged defects at the GBs and surface, including undercoordinated halide species and undercoordinated Pb(2+) ions, thereby effectively inhibiting the charge trapping/recombination centers. Two-dimensional confocal-fluorescence mapping images provide a visualized sight into the significantly suppressed nonradiative recombination and the prolonged carrier lifetime. It is suggested that the 4-GBACl additive plays multiple roles in grain cross-linking to regulate crystallization, distinctly reducing the trap-state density, ion migration inhibition, and moisture barrier in CsPbI(2)Br films. Consequently, the 4-GBACl-treated device exhibits a champion power conversion efficiency (PCE) of 15.59% accompanied with a considerably improved V(oc) of 1.28 V and maintains 88% of the initial PCE value after 1200 h aging under 20% relative humidity. FAU - Li, Hui AU - Li H AUID- ORCID: 0000-0003-0440-921X AD - Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, P. R.China. FAU - Hao, Xiaotao AU - Hao X AUID- ORCID: 0000-0002-0197-6545 AD - State Key Laboratory of Crystal Materials, School of Physics, Shandong University, Jinan 250100, P. R.China. FAU - Chang, Bohong AU - Chang B AD - Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, P. R.China. FAU - Li, Zihao AU - Li Z AD - Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, P. R.China. FAU - Wang, Lian AU - Wang L AD - Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, P. R.China. FAU - Pan, Lu AU - Pan L AD - Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, P. R.China. FAU - Chen, Xihan AU - Chen X AUID- ORCID: 0000-0001-7907-2549 AD - Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, P. R.China. FAU - Yin, Longwei AU - Yin L AUID- ORCID: 0000-0003-3768-6846 AD - Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, P. R.China. LA - eng PT - Journal Article DEP - 20210818 PL - United States TA - ACS Appl Mater Interfaces JT - ACS applied materials & interfaces JID - 101504991 SB - IM OTO - NOTNLM OT - CsPbI2Br OT - [PbX6]4- octahedron OT - charge trapping OT - defect passivation OT - stability EDAT- 2021/08/19 06:00 MHDA- 2021/08/19 06:01 CRDT- 2021/08/18 08:43 PHST- 2021/08/19 06:00 [pubmed] PHST- 2021/08/19 06:01 [medline] PHST- 2021/08/18 08:43 [entrez] AID - 10.1021/acsami.1c06533 [doi] PST - ppublish SO - ACS Appl Mater Interfaces. 2021 Sep 1;13(34):40489-40501. doi: 10.1021/acsami.1c06533. Epub 2021 Aug 18.