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Ca-triggered allosteric catalysts crosstalk with cellular redox systems through their foldase- and reductase-like activities.
Commun Chem
March 2025
Department of Chemistry, School of Science, Tokai University, 4-1-1 Kitakaname, Hiratsuka-shi, Kanagawa, Japan.
Effective chemical catalysts can artificially control intracellular metabolism. However, in conventional catalytic chemistry, activity and cytotoxicity have a trade-off relationship; thus, driving catalysts in living cells remains challenging. To overcome this critical issue at the interface between catalytic chemistry and biology, we developed cell-driven allosteric catalysts that exert catalytic activity at specific times.
View Article and Find Full Text PDFSelectively Deoxygenative Deuteration of Aldehydes by Superwetting Porous Carbon-Supported Palladium Catalysts.
Angew Chem Int Ed Engl
March 2025
State Key Laboratory of Fine Chemicals, Frontier Science Center for Smart Materials, Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, and School of Chemical Engineering, Dalian University of Technology, Dalian, Liaoning, 116024, P.R. China.
We present a method of deoxygenative deuteration of aldehydes (DDA) over heterogeneously superwetting porous carbon-supported palladium catalyst (Pd/SPC), which is efficient for the synthesis of deuterated aromatic compounds with -CD group. Exemplified by the DDA reaction of 2-naphthaldehyde (2-NAL) to 2-methylnaphthalene (2-MNE), the total deuterium incorporation radio in the resultant aromatic hydrocarbons was higher than 95% and the selectivity toward 2-MNE-d reached 87%. The impressed catalytic activity was found relevant to the combined effect of surface wettability and the electron-rich properties of Pd species of this kind of heterogeneous Pd/SPC catalyst.
View Article and Find Full Text PDFHigh Entropy Oxide-Polyoxometalate Sub-1 nm Hetero-Nanowires as Cathode Catalysts in Li-O Batteries.
J Am Chem Soc
March 2025
Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing 100084, China.
It is desirable for lithium-oxygen batteries (LOBs) to fabricate the cathode catalysts with high catalytic activity and stability. High entropy oxide (HEO) sub-1 nm nanowires (SNWs) with the nearly 100% active site exposure and intrinsic stability are doubtless one of the best candidates. Herein, under a mild solvothermal condition, by incorporating phosphomolybdic acid (PMA) into multimetal oxide reaction system, a series of HEO-PMA SNWs are successfully prepared, where the variety of metal oxides is adjustable from mono component to six components.
View Article and Find Full Text PDFHighly Selective Electrocatalytic 1,4-NADH Regeneration Based on Host-Guest Recognition Mediated by Cucurbit[8]uril on NiO.
Angew Chem Int Ed Engl
February 2025
State Key Laboratory of Fine Chemicals, Frontier Science Center for Smart Materials, School of Chemical Engineering, Dalian University of Technology, Dalian, Liaoning, 116024, China.
Efficient regeneration of nicotinamide adenine dinucleotide (NADH) cofactors, particularly 1,4-NADH, is crucial for advancing oxidoreductase catalysis. Electrocatalysis provides a promising route for 1,4-NADH regeneration, but an expensive catalyst, typically a rhodium organometallic complex, is frequently required to guarantee the high selectivity of 1,4-NADH, significantly limiting its large-scale application. Herein, inspired by the catalytic pocket and enzyme-substrate interaction in nature, a direct electrochemical 1,4-NADH regeneration route was designed by modification of the surface of nickel oxide (NiO) with cucurbit[8]uril (CB[8]) (denoted as CB[8]-NiO).
View Article and Find Full Text PDFIdentification and Quantification of Al Pairs and Their Impact on Dealumination in Zeolites.
J Am Chem Soc
February 2025
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, China.
Understanding the precise quantity and spatial distribution of paired aluminum (Al) sites in zeolite catalysts is crucial, as they significantly impact the catalytic performance via synergistic effects and long-term stability. In this study, a novel strategy by employing divalent cation titration with varying cation sizes, in combination with advanced quantitative H NMR and H-H homonuclear correlation techniques, has been developed to accurately identify and classify three distinct types of Al pairs. These include two types of Al pairs aligned along six-membered rings (6-MRs) and 10-membered rings (10-MRs), the latter of which are essentially composed of Al atoms located in different 6-MR or 5-MR.
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