To relieve the green gas emission and involve the carbon neutral cycle, electrochemical reduction of CO attracts more and more attention. Herein, a biatomic site catalyst of Cu-Fe coordinated with the nitrogen, which is doped in the carbon matrix (denoted as Cu-Fe-N -C), is designed. The as-obtained Cu-Fe-N -C exhibits higher performance than that of Cu-N-C and Fe-N-C, owing to bimetallic sites, proving synergistic functions based on different molecules and their interfaces. Cu-Fe-N -C shows high selectivity toward CO, with high Faradaic efficiency (98% at -0.7 V), and maintaining 98% of its initial selectivity after 10 h electrolysis. The experimental results and theoretical calculations reveal that the synergistic catalysis of different metallic sites enlarges the adsorption enthalpy of CO , reducing the activation energy result in generating high selectivity, activity, stability, and low impedance.
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http://dx.doi.org/10.1002/smll.202006951 | DOI Listing |
Anal Methods
January 2025
Jiangxi University of Chinese Medicine, Nan Chang, Jiangxi 330004, China.
This study reports a novel ratiometric fluorescence sensor based on a tetraphenylethylene-bipyridine covalent organic framework (TPE-Bpy-COF) for the sensitive detection of Cu, leveraging the unique coordination properties of the bipyridine moieties. The interaction between Cu and the nitrogen atoms in the bipyridine units induces fluorescence quenching at 500 nm through an efficient host-guest electron transfer mechanism, where excited-state electrons from the COF framework are transferred to the vacant orbitals of Cu. Upon excitation at 410 nm, the sensor exhibits a primary emission peak at 500 nm, which is quenched in the presence of Cu, while an overtone peak at 820 nm remains stable, serving as an internal reference for ratiometric measurements and significantly enhancing the accuracy and reliability of the sensor.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Metallurgical and Materials Enginerring, Colorado School of Mines, Golden, Colorado 80401, United States.
The sizes of the basins of attraction on the potential energy surface are helpful indicators in determining the experimental synthesizability of metastable phases. In principle, these basins can be controlled with changes in thermodynamic conditions such as composition, pressure, and surface energy. Herein, we use random structure sampling to computationally study how alloying smoothly perturbs basin of attraction sizes.
View Article and Find Full Text PDFHeliyon
January 2025
Department of Geography & Environmental Study, Arba Minch University, Ethiopia.
Crop farming by smallholder farmers of Ethiopia and Sile Watershed is practiced based on commonsense experiences of farmers. This study was targeted to evaluate the suitability of land for the production of four major crops in Sile Watershed. Data were acquired from sources such as climate data (from CHRS data portal CRU TSv.
View Article and Find Full Text PDFSci Rep
January 2025
Florida State University, Tallahassee, FL, 32306-2400, USA.
Sphagnum-dominated bogs are climatically impactful systems that exhibit two puzzling characteristics: CO:CH ratios are greater than those predicted by electron balance models and C decomposition rates are enigmatically slow. We hypothesized that Maillard reactions partially explain both phenomena by increasing apparent CO production via eliminative decarboxylation and sequestering bioavailable nitrogen (N). We tested this hypothesis using incubations of sterilized Maillard reactants, and live and sterilized bog peat.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China.
The comprehensive understanding of the effect of the chemical environment surrounding active sites on the pathway for the electrochemical carbon dioxide reduction reaction (eCORR) is essential for the development of advanced catalysts for large-scale applications. Based on a series of model catalysts engineered by the coordination of copper ions with various isomers of phenylenediamine [i.e.
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