Currently, more than 86% of global energy consumption is still mainly dependent on traditional fossil fuels, which causes resource scarcity and even emission of high amounts of carbon dioxide (CO2), resulting in a severe “Greenhouse effect.” Considering this situation, the concept of “carbon neutrality” has been put forward by 125 countries one after another. To achieve the goals of “carbon neutrality,” two main strategies to reduce CO2 emissions and develop sustainable clean energy can be adopted. Notably, these are crucial for the synthesis of advanced single-atom catalysts (SACs) for energy-related applications. In this review, we highlight unique SACs for conversion of CO2 into high-efficiency carbon energy, for example, through photocatalytic, electrocatalytic, and thermal catalytic hydrogenation technologies, to convert CO2 into hydrocarbon fuels (CO, CH4, HCOOH, CH3OH, and multicarbon [C2+] products). In addition, we introduce advanced energy conversion technologies and devices to replace traditional polluting fossil fuels, such as photocatalytic and electrocatalytic water splitting to produce hydrogen energy and a high-efficiency oxygen reduction reaction (ORR) for fuel cells. Impressively, several representative examples of SACs (including d-, ds-, p-, and f-blocks) for CO2 conversion, water splitting to H2, and ORR are discussed to describe synthesis methods, characterization, and corresponding catalytic activity. Finally, this review concludes with a description of the challenges and outlooks for future applications of SACs in contributing toward carbon neutrality. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/cey2.194

Single‐atom catalysis for carbon neutrality

Ligand-free Synthesis of Noble Metal Nanocatalysts for Electrocatalysis

Co-catalytic metal–support interactions in single-atom electrocatalysts

Single-atom catalysts (SACs) have attracted considerable attention in heterogeneous catalysis because of their well-defined active sites, maximum atomic utilization efficiency, and unique unsaturated coordinated structures. However, their effectiveness is limited to reactions requiring active sites containing multiple metal atoms. Furthermore, the loading amounts of single-atom sites must be restricted to prevent aggregation, which can adversely affect the catalytic performance despite the high activity of the individual atoms. The introduction of nanoscale metal particles (NMPs) into SACs (NMP-SACs) has proven to be an efficient approach for improving their catalytic performance. A comprehensive review is urgently needed to systematically introduce the synthesis, characterization, and application of NMP-SACs and the mechanisms behind their superior catalytic performance. This review first presents and classifies the different mechanisms through which NMPs enhance the performance of SACs. It then summarizes the currently reported synthetic strategies and state-of-the-art characterization techniques of NMP-SACs. Moreover, their application in electro/thermo/photocatalysis, and the reasons for their superior performance are discussed. Finally, we address the challenges and perspectives of NMP-SACs for the future design of advanced catalysts. This article is protected by copyright. All rights reserved.

Nanoscale Metal Particle Modified Single-Atom Catalyst: Synthesis, Characterization, And Application.

Electrochemical CO2 reduction reaction (CO2RR) offers a promising approach to close the anthropogenic carbon cycle and store intermittent renewable energy in fuels or chemicals. On the path to commercializing this technology, achieving the long‐term operation stability is a central requirement but still confronts challenges. This motivates to organize the present review to systematically discuss the stability issue of CO2RR. This review starts from the fundamental understanding on the destabilization mechanisms of CO2RR, with focus on the degradation of electrocatalyst and change of reaction microenvironment during continuous electrolysis. Subsequently, recent efforts on catalyst design to stabilize the active sites are summarized, where increasing atomic binding strength to resist surface reconstruction is highlighted. Next, the optimization of electrolysis system to enhance the operation stability by maintaining reaction microenvironment especially mitigating flooding and carbonate problems is demonstrated. The manipulation on operation conditions also enables to prolong CO2RR lifespan through recovering catalytically active sites and mass transport process. This review finally ends up by indicating the challenges and future opportunities.

Stability Issues in Electrochemical CO2 Reduction: Recent Advances in Fundamental Understanding and Design Strategies.

Electrochemical CO2 reduction reaction (CO2RR) offers a practical solution to current global greenhouse effect by converting excessive CO2 into value-added chemicals or fuels. Noble metal-based nanomaterials have been considered as efficient catalysts for the CO2RR owing to their high catalytic activity, long-term stability and superior selectivity to targeted products. On the other hand, they are usually loaded on different support materials in order to minimize their usage and maximize the utilization because of high price and limited reserve. The strong metal-support interaction (MSI) between the metal and substrate plays an important role in affecting the CO2RR performance. In this review, we mainly focus on different types of support materials (e.g., oxides, carbons, ligands, alloys and metal carbides) interacting with noble metal as electrocatalysts for CO2RR. Moreover, the positive effects about MSI for boosting the CO2RR performance via regulating the adsorption strength, electronic structure, coordination environment and binding energy are presented. Lastly, emerging challenges and future opportunities on noble metal electrocatalysts with strong MSI are discussed.

Metal-support interactions in designing noble metal-based catalysts for electrochemical CO 2 reduction: Recent advances and future perspectives

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Metal-support interactions in designing noble metal-based catalysts for electrochemical CO 2 reduction: Recent advances and future perspectives