A three-dimensional quantum dot network stabilizes perovskite solids via hydrostatic strain(Elsevier BV, 2023-11) Liu, Yuan; Zhu, Tong; Grater, Luke; Chen, Hao; dos Reis, Roberto; Maxwell, Aidan; Cheng, Matthew; Dong, Yitong; Teale, Sam; Leontowich, Adam F.G.; Kim, Chang Yong; Chan, Phoebe Tsz shan; Wang, Mingcong; Paritmongkol, Watcharaphol; Gao, Yajun; Park, So Min; Xu, Jian; Khan, Jafar Iqbal; Laquai, Frédéric; Walker, Gilbert C.; Dravid, Vinayak P.; Chen, Bin; Sargent, Edward H.; KAUST Catalysis Center (KCC); KAUST Solar Center (KSC); Physical Science and Engineering (PSE) Division; Material Science and Engineering Program; Applied Physics; Department of Electrical and Computer Engineering, University of Toronto, 35 St. George Street, Toronto, ON M5S 1A4, Canada; Department of Electrical and Computer Engineering, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208, USA; Department of Materials Science and Engineering, Northwestern University, Evanston, IL 60208, USA; The NUANCE Center, Northwestern University, Evanston, IL 60208, USA; International Institute of Nanotechnology, Northwestern University, Evanston, IL 60208, USA; Department of Chemistry and Biochemistry, University of Oklahoma, Norman, OK 73019, USA; Canadian Light Source, 44 Innovation Boulevard, Saskatoon, SK S7N 2V3, Canada; Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON M5S 3H6, Canada; Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208, USA
Compressive strain engineering improves perovskite stability. Two-dimensional compressive strain along the in-plane direction can be applied to perovskites through the substrate; however, this in-plane strain results in an offsetting tensile strain perpendicular to the substrate, linked to the positive Poisson ratio of perovskites. Substrate-induced strain engineering has not yet resulted in state-of-the-art operational stability. Here, we seek instead to implement hydrostatic strain in perovskites by embedding lattice-mismatched perovskite quantum dots (QDs) into a perovskite matrix. QD-in-matrix perovskites show a homogeneously strained lattice as evidenced by grazing-incidence X-ray diffraction. We fabricate mixed-halide wide-band-gap (Eg; 1.77 eV) QD-in-matrix perovskite solar cells that maintain >90% of their initial power conversion efficiency (PCE) after 200 h of one-sun operation at the maximum power point (MPP), a significant improvement relative to matrix-only devices, which lose 10% (relative) of their initial PCE after 5 h of MPP tracking.
Functional decoration on a regenerable bifunctional porous covalent organic framework probe for rapid detection and adsorption of copper ions(Springer Science and Business Media LLC, 2023-11-25) Li, Yu Long; Jin, Xi Lang; Ma, Yi Ting; Liu, Jing Rui; Raziq, Fazal; Zhu, Peng Yuan; Deng, Zhi Feng; Zhou, Hong Wei; Chen, Wei Xing; Huang, Wen Huan; KAUST Catalysis Center (KCC); Physical Science and Engineering (PSE) Division; School of Materials and Chemical Engineering, Xi’an Technological University, Xi’an, 710021, China; Yulin Boyi-Jingking Research Institute of Industrial Technology Development Research, Yulin, 719054, China; Key Laboratory of Chemical Additives for China National Light Industry, College of Chemistry and Chemical Engineering, Shaanxi University of Science and Technology, Xi’an, 710021, China; National and Local Joint Engineering Laboratory for Slag Comprehensive Utilization and Environmental Technology, School of Materials Science and Engineering, Shaanxi University of Technology, Hanzhong, 723001, China
Abstract: Developing fluorescence porous probe for detecting and eliminating Cu2+ contamination in water or biosystem is an essential research project that has attracted considerable attention. However, improving the fluorescence detecting efficiency while enhancing the adsorption capacity of the porous probe is of great challenge. Herein, a bifunctional two-dimensional imine-based porous covalent organic framework (TTP-COF) probe was designed and synthesized from 1,3,5-tris (4-aminophenyl) benzene (TAPB) and 2,4,6-Triformylphloroglucinol (TP) ligand. TTP-COF displayed rapid detection of Cu2+ (limit of detection (LOD) = 10 nmol·L−1 while achieving a high adsorption capacity of 214 mg·g−1 (pH = 6) at room temperature with high reusability (> 5 cycles). The key roles and contributions of high π-conjugate and delocalized electrons in TABP and functional –OH groups in TP were proved. More importantly, the fluorescence quenching mechanism of TTP-COF was studied by density functional theory theoretical calculations, revealing the crucial role of intramolecular hydrogen bonds among C=N and –OH groups and the blocking of the excited state intramolecular proton transfer process in detecting process of Cu2+. Graphical abstract: [Figure not available: see fulltext.].
Correlating Structural Disorder in Metal (Oxy)hydroxides and Catalytic Activity in Electrocatalytic Oxygen Evolution(Wiley, 2023-12) Zuo, Shouwei; Wu, Zhipeng; Zhang, Guikai; Chen, Cailing; Ren, Yuanfu; Zheng, Lirong; Zhang, Jing; Han, Yu; Zhang, Huabin; King Abdullah University of Science and Technology PSE Thuwal 23955-6900 Jeddah SAUDI ARABIA; King Abdullah University of Science and Technology PSE SAUDI ARABIA; King Abdullah University of Science and Technology Materials Science and Engineering Thuwal 23955-6900, Jeddah SAUDI ARABIA; KAUST Catalysis Center (KCC); Physical Science and Engineering (PSE) Division; Advanced Membranes and Porous Materials Research Center; Chemical Science Program; Graduate Affairs; Scholarship Programs; Office of the Provost; Material Science and Engineering Program; Chinese Academy of Sciences Institute of High Energy Physics CHINA
Understanding the correlation between the structural evolution of electrocatalysts and their catalytic activity is both essential and challenging. In this study, we investigate this correlation in the context of the oxygen evolution reaction (OER) by examining the influence of structural disorder during/after the dynamic structural evolution on their OER activity of Fe-Ni (oxy)hydroxide catalysts using operando X-ray absorption spectroscopy, alongside other experiments and theoretical calculations. The Debye-Waller factors obtained from extended X-ray absorption fine structure analyses reflect the degree of structural disorder and exhibit a robust correlation with the intrinsic OER activities of the electrocatalysts. Enhanced OER activity of in-situ generated metal (oxy)hydroxides derived from different pre-catalysts is linked to increased structural disorder, offering a promising approach for designing efficient OER electrocatalysts. This strategy may inspire similar investigations in related electrocatalytic energy-conversion systems.
O–H bond activation of β,γ-unsaturated oximes via hydrogen atom transfer (HAT) and photoredox dual catalysis(Royal Society of Chemistry (RSC), 2023) Yi, Liang; Zhu, Chen; Chen, Xiangyu; Yue, Huifeng; Ji, Tengfei; Ma, Yiqiao; Cao, Yuanyuan; Kancherla, Rajesh; Rueping, Magnus; KAUST Catalysis Center (KCC); Physical Science and Engineering (PSE) Division; Chemical Science Program; Institute of Organic Chemistry, RWTH Aachen University, Landoltweg 1, D-52074 Aachen, Germany
Activating O–H bonds in β,γ-unsaturated oximes is challenging due to high redox potential. Our method combines HAT and photoredox catalysis to allow the synthesis of diverse heterocycles using various radical acceptors. Mechanistic studies support the HAT process in O–H bond activation.
Catalyst switch strategy enabled a single polymer with five different crystalline phases(Springer Science and Business Media LLC, 2023-11-20) Zhang, Pengfei; Ladelta, Viko; Abou-Hamad, Edy; Müller, Alejandro J.; Hadjichristidis, Nikos; Polymer Synthesis Laboratory, KAUST Catalysis Center, Chemistry Program, Physical Sciences and Engineering Division, King Abdullah University of Science and Technology (KAUST), Thuwal, 23955, Saudi Arabia; Chemical Science Program; Physical Science and Engineering (PSE) Division; KAUST Catalysis Center (KCC); NMR; Imaging and Characterization Core Lab; Department of Polymers and Advanced Materials, Physics, Chemistry and Technology, Faculty of Chemistry, University of the Basque Country UPV/EHU, Paseo Manuel de Lardizabal 3, 20018, Donostia-San Sebastián, Spain
Well-defined multicrystalline multiblock polymers are essential model polymers for advancing crystallization physics, phase separation, self-assembly, and improving the mechanical properties of materials. However, due to different chain properties and incompatible synthetic methodologies, multicrystalline multiblock polymers with more than two crystallites are rarely reported. Herein, by combining polyhomologation, ring-opening polymerization, and catalyst switch strategy, we synthesized a pentacrystalline pentablock quintopolymer, polyethylene-b-poly(ethylene oxide)-b-poly(ε-caprolactone)-b-poly(L-lactide)-b-polyglycolide (PE-b-PEO-b-PCL-b-PLLA-b-PGA). The fluoroalcohol-assisted catalyst switch enables the successful incorporation of a high melting point polyglycolide block into the complex multiblock structure. Solid-state nuclear magnetic resonance spectroscopy, X-ray diffraction, and differential scanning calorimetry revealed the existence of five different crystalline phases.