Conversion of carbon monoxide (CO), a major one-carbon product of carbon dioxide (CO) reduction, into value-added multicarbon species is a challenge to addressing global energy demands and climate change. Here we report a modular synthetic approach for aqueous electrochemical CO reduction to carbon-carbon coupled products via self-assembly of supramolecular cages at molecular-materials interfaces. Heterobimetallic cavities formed by face-to-face coordination of thiol-terminated metalloporphyrins to copper electrodes through varying organic struts convert CO to C2 products with high faradaic efficiency (FE = 83% total with 57% to ethanol) and current density (1.34 mA/cm) at a potential of -0.40 V vs RHE. The cage-functionalized electrodes offer an order of magnitude improvement in both selectivity and activity for electrocatalytic carbon fixation compared to parent copper surfaces or copper functionalized with porphyrins in an edge-on orientation.
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http://dx.doi.org/10.1021/acscentsci.7b00316 | DOI Listing |
Adv Sci (Weinh)
January 2025
Institute of Molecular Science, University of Valencia, c/Catedrático José Beltrán Martínez 2, Paterna, 46980, Valencia, Spain.
Energy transfer processes in nanohybrids are at the focal point of conceptualizing, designing, and realizing novel energy-harvesting systems featuring nanocrystals that absorb photons and transfer their energy unidirectionally to surface-immobilized functional dyes. Importantly, the functionality of these dyes defines the ultimate application. Herein, CsPbBr perovskite nanocrystals (NCs) are interfaced with zinc phthalocyanine (ZnPc) dyes featuring carboxylic acid.
View Article and Find Full Text PDFJ Phys Chem Lett
January 2025
Molecular Materials and Nanosystems & Institute for Complex Molecular Systems, Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, The Netherlands.
Reducing nonradiative recombination is crucial for minimizing voltage losses in metal-halide perovskite solar cells and achieving high power conversion efficiencies. Photoluminescence spectroscopy on complete or partial perovskite solar cell stacks is often used to quantify and disentangle bulk and interface contributions to nonradiative losses. Accurately determining the intrinsic loss in a perovskite layer is key to analyzing the origins of nonradiative recombination and developing defect engineering strategies.
View Article and Find Full Text PDFNat Commun
January 2025
Molecular Materials and Nanosystems, Institute of Complex Molecular Systems, Eindhoven University of Technology, partner of Solliance, P.O. Box 513, 5600 MB, Eindhoven, The Netherlands.
All-perovskite tandem photovoltaics are a potentially cost-effective technology to power chemical fuel production, such as green hydrogen. However, their application is limited by deficits in open-circuit voltage and, more challengingly, poor operational stability of the photovoltaic cell. Here we report a laboratory-scale solar-assisted water-splitting system using an electrochemical flow cell and an all-perovskite tandem solar cell.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
College of Chemistry, Zhengzhou University, Zhengzhou 450001, P. R. China.
Programming and synthesizing bifunctional materials for regulating the output of triboelectric nanogenerators (TENGs) and their photocatalytic efficiency is a promising strategy for energy harvesting to build self-powered systems. Herein, we tackle this challenge by introducing metal-organic frameworks (MOFs) as molecular catalysts and triboelectric layers for self-powered photocatalytic systems. A zeolite-like mixed-valence MOF () and a ladder-structured MOF () were obtained through structural transformation.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2024
State Key Laboratory of Molecular Engineering of Polymers, Fudan University, Shanghai 200433, China.
In recent years, field-effect transistor (FET) sensing technology has attracted significant attention owing to its noninvasive, label-free, real-time, and user-friendly detection capabilities. Owing to the large specific surface area, high flexibility, and excellent conductivity of two-dimensional (2D) materials, FET biosensors based on 2D materials have demonstrated unique potential in biomarker analysis and healthcare applications, driving continuous innovation and transformation in the field. Here, we review recent trends in the development of 2D FET biosensors based on key performance metrics and main characteristics, and we also discuss structural designs and modification strategies for biosensing devices utilizing graphene, transition metal dichalcogenides, black phosphorus, and other 2D materials to enhance key performance metrics.
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