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• W4226051141 endingPage "134969" @default.
• W4226051141 startingPage "134969" @default.
• W4226051141 abstract "• Uniform composition-controlled Cu x Pd 100-x alloy NWs are prepared for NO 3 RR. • Cu 28 Pd 72 NWs deliver an unprecedented N 2 selectivity of 75.9 ± 5.2% in product. • N 2 formation is kinetically favored via a pathway of NO 2 * → NO* → N* → N 2 * on Pd. • Contiguous surface Pd ensemble with specific size is the key to high N 2 selectivity. • Cu serves to initiate NO 3 – –NO 2 * conversion and lower H ads coverage on Pd ensemble. Selective electrocatalytic nitrate reduction reaction (NO 3 RR) to dinitrogen (N 2 ) is essential to nitrogen-cycle management and environmental sustainability. Palladium-based nanomaterials were extensively studied as NO 3 RR catalysts, but only delivered limited N 2 selectivity (<50%, NH 3 dominated the product). Here we report that, by tuning bimetallic composition of CuPd alloy nanowires, the Cu 28 Pd 72 nanowires deliver a near-unit conversion of NO 3 – -N and an unprecedented N 2 product selectivity of 75.9 ± 5.2% in treating 22.5 mg L −1 NO 3 – -N solution at −0.80 V vs. Ag/AgCl. Combining in-situ spectrometric measurements and theoretical calculations, we demonstrate that the contiguous Pd ensemble with a specific size at catalyst surface is essential to the N 2 formation via a kinetically-favored pathway of NO 2 * → NO* → N* → N 2 *. Alloying Pd with Cu is indispensable as Cu contributes to the N*-N* pairing by initiating the NO 3 – –NO 2 * conversion and lowering the H ads coverage on catalyst. This work discloses the key surface atomic structure for N 2 formation, and provides a guideline for the design of efficient NO 3 RR catalyst that enables selective NO 3 – –N 2 conversion." @default.
• W4226051141 created "2022-05-05" @default.
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• W4226051141 date "2022-05-01" @default.
• W4226051141 modified "2023-10-01" @default.
• W4226051141 title "Electrocatalytic nitrate reduction on bimetallic Palladium-Copper Nanowires: Key surface structure for selective dinitrogen formation" @default.
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• W4226051141 doi "https://doi.org/10.1016/j.cej.2022.134969" @default.
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