Accelerated Transfer and Spillover of Carbon Monoxide through Tandem Catalysis for Kinetics‐boosted Ethylene Electrosynthesis

Abstract

Cu-based catalysts have been widely applied in electroreduction of carbon dioxide (CO 2 ER) to produce multicarbon (C 2 + ) feedstocks (e.g., C 2 H 4 ). However, the high energy barriers for CO 2 activation on the Cu surface is a challenge for a high catalytic efficiency and product selectivity. Herein, we developed an in situ *CO generation and spillover strategy by engineering single Ni atoms on a pyridinic N-enriched carbon support with a sodalite (SOD) topology (Ni-SOD/NC) that acted as a donor to feed adjacent Cu nanoparticles (NPs) with *CO intermediate. As a result, a high C 2 H 4 selectivity of 62.5 % and an industrial-level current density of 160 mA cm À 2 at a low potential of À 0.72 V were achieved. Our studies revealed that the isolated NiN 3 active sites with adjacent pyridinic N species facilitated the *CO desorption and the massive *CO intermediate released from Ni-SOD/NC then overflowed to Cu NPs surface to enrich the *CO coverage for improving the selectivity of CO 2 ER to C 2 H 4 .

Accelerating industrial-level CO2electroreduction kinetics on isolated zinc centersviasulfur-boosted bicarbonate dissociation

“…Converting CO 2 into valuable chemicals through renewable electricity-driven CO 2 electroreduction reaction (CO 2 ER) offers a promising approach to mitigate the over-accumulated CO 2 in the atmosphere. To date, substantial endeavors have been made to catalyze CO 2 into CO using a single metal atom supported on nitrogen-doped carbon (M-SAs-N–C) 1–6 because produced gaseous CO can be directly separated from the aqueous CO 2 ER system and further used as the feedstock of syngas to produce fuels via Fischer-Tropsch synthesis. 7 Despite certain progress in M-SAs-N–C catalyzed CO 2 ER, the sluggish reaction kinetics of the proton-coupled electron transfer (PCET) process in the electrocatalysis of CO 2 reduction largely limits its practical applications.…”

Tuning the Microenvironment in Monolayer MgAl Layered Double Hydroxide for CO2‐to‐Ethylene Electrocatalysis in Neutral Media

“…Furthermore, the Cu 2p peaks at 935.3 and 954.6 eV were observed, accompanied by satellite peaks at around 943, 945, and 964 eV assigned to Cu II 2p peaks, which could result from slight oxidation in the air. [25] Meanwhile, XPS spectra of Mg and Al elements were also applied to investigate the chemical state of MgAl-LDH (Figure S10). The characteristic peaks attributed to MgÀ O and AlÀ O remain unchanged after reaction.…”

Energy-Efficient Ammonia Synthesis from Nitrate via CoNi Alloys Incorporated in Carbon Frameworks

“…Transitional metals (Cu, Co, Ni, and Fe) have been used as catalysts for nitrate reduction. ,, However, they usually catalyze at highly negative applied potentials (such as < −0.4 V vs RHE), which is energetically inefficient for future applications. Designing heterostructures such as metal/carbon hybrids can efficiently facilitate electron transfer and endow the structures with a large number of stable electrochemical active sites. , Metal–organic frameworks (MOFs) have attracted substantial interest owing to their tailorable derived heterostructures, compositional flexibility and the ability to form porous carbon frameworks. − These merits make the synthesis of hybrids comprising alloying metals highly feasible. Noteworthy, MOF with cobalt ions distributed (ZIF-67) has drawn considerable attention owing to the high electrocatalytic activity of its Co-based yolk–shell structure. , Further, the introduction of heteroatoms in metal catalysts can modulate the electronic structure, which is essential for improving the electrocatalytic activity.…”