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The electrochemical CO₂reduction reaction (CO₂RR) is a promising approach to achieving sustainable electrical‐to‐chemical energy conversion and storage while decarbonizing the emission‐heavy industry. The carbon‐supported, nitrogen‐coordinated, and atomically dispersed metal sites are effective catalysts for CO generation due to their high activity, selectivity, and earth abundance. Here, we discuss progress, challenges, and opportunities for designing and engineering atomic metal catalysts from single to dual metal sites. Engineering single metal sites using a nitrogen‐doped carbon model was highlighted to exclusively study the effect of carbon particle sizes, metal contents, and M−N bond structures in the form of MN₄moieties on catalytic activity and selectivity. The structure‐property correlation was analyzed by combining experimental results with theoretical calculations to uncover the CO₂to CO conversion mechanisms. Furthermore, dual‐metal site catalysts, inheriting the merits of single‐metal sites, have emerged as a new frontier due to their potentially enhanced catalytic properties. Designing optimal dual metal site catalysts could offer additional sites to alter the surface adsorption to CO₂and various intermediates, thus breaking the scaling relationship limitation and activity‐stability trade‐off. The CO₂RR electrolysis in flow reactors was discussed to provide insights into the electrolyzer design with improved CO₂utilization, reaction kinetics, and mass transport.

The electrochemical CO₂reduction reaction (CO₂RR) is a promising approach to achieving sustainable electrical‐to‐chemical energy conversion and storage while decarbonizing the emission‐heavy industry. The carbon‐supported, nitrogen‐coordinated, and atomically dispersed metal sites are effective catalysts for CO generation due to their high activity, selectivity, and earth abundance. Here, we discuss progress, challenges, and opportunities for designing and engineering atomic metal catalysts from single to dual metal sites. Engineering single metal sites using a nitrogen‐doped carbon model was highlighted to exclusively study the effect of carbon particle sizes, metal contents, and M−N bond structures in the form of MN₄moieties on catalytic activity and selectivity. The structure‐property correlation was analyzed by combining experimental results with theoretical calculations to uncover the CO₂to CO conversion mechanisms. Furthermore, dual‐metal site catalysts, inheriting the merits of single‐metal sites, have emerged as a new frontier due to their potentially enhanced catalytic properties. Designing optimal dual metal site catalysts could offer additional sites to alter the surface adsorption to CO₂and various intermediates, thus breaking the scaling relationship limitation and activity‐stability trade‐off. The CO₂RR electrolysis in flow reactors was discussed to provide insights into the electrolyzer design with improved CO₂utilization, reaction kinetics, and mass transport.

Unrestrained anthropogenic activities have severely disrupted the global natural nitrogen cycle, causing numerous energy and environmental issues. Electrocatalytic nitrogen transformation is a feasible and promising strategy for achieving a sustainable nitrogen economy. Synergistically combining multiple nitrogen reactions can realize efficient renewable energy storage and conversion, restore the global nitrogen balance, and remediate environmental crises. Here, we provide a unique aspect to discuss the intriguing nitrogen electrochemistry by linking three essential nitrogen‐containing compounds (i.e., N₂, NH₃, and NO₃⁻) and integrating four essential electrochemical reactions, i.e., the nitrogen reduction reaction (N₂RR), nitrogen oxidation reaction (N₂OR), nitrate reduction reaction (NO₃RR), and ammonia oxidation reaction (NH₃OR). This minireview also summarizes the acquired knowledge of rational catalyst design and underlying reaction mechanisms for these interlinked nitrogen reactions. We further underscore the associated clean energy technologies and a sustainable nitrogen‐based economy.

Unrestrained anthropogenic activities have severely disrupted the global natural nitrogen cycle, causing numerous energy and environmental issues. Electrocatalytic nitrogen transformation is a feasible and promising strategy for achieving a sustainable nitrogen economy. Synergistically combining multiple nitrogen reactions can realize efficient renewable energy storage and conversion, restore the global nitrogen balance, and remediate environmental crises. Here, we provide a unique aspect to discuss the intriguing nitrogen electrochemistry by linking three essential nitrogen‐containing compounds (i.e., N₂, NH₃, and NO₃⁻) and integrating four essential electrochemical reactions, i.e., the nitrogen reduction reaction (N₂RR), nitrogen oxidation reaction (N₂OR), nitrate reduction reaction (NO₃RR), and ammonia oxidation reaction (NH₃OR). This minireview also summarizes the acquired knowledge of rational catalyst design and underlying reaction mechanisms for these interlinked nitrogen reactions. We further underscore the associated clean energy technologies and a sustainable nitrogen‐based economy.

Electrochemical CO₂reduction offers a compelling route to mitigate atmospheric CO₂concentration and store intermittent renewable energy in chemical bonds. Beyond C₁, C₂₊feedstocks are more desirable due to their higher energy density and more significant market need. However, the CO₂‐to‐C₂₊reduction suffers from significant barriers of CC coupling and complex reaction pathways. Due to remarkable tunability over morphology/pore architecture along with great feasibility of functionalization to modify the electronic and geometric structures, carbon materials, serving as active components, supports, and promoters, provide exciting opportunities to tune both the adsorption properties of intermediates and the local reaction environment for the CO₂reduction, offering effective solutions to enable CC coupling and steer C₂₊evolution. However, general design principles remain ambiguous, causing an impediment to rational catalyst refinement and application thrusts. This review clarifies insightful design principles for advancing carbon materials. First, the current performance status and challenges are discussed and effective strategies are outlined to promote C₂₊evolution. Further, the correlation between the composition, structure, and morphology of carbon catalysts and their catalytic behavior is elucidated to establish catalytic mechanisms and critical factors determining C₂₊performance. Finally, future research directions and strategies are envisioned to inspire revolutionary advancements.