Mg–CO2 battery as a promising strategy for CO2 conversion and utilization is challenging, owing to the sluggish kinetics of CO2 reduction reaction (CO2RR) and the waste of the sacrificial Mg anode. Herein, by elaborately designing a highly selective Ni NPs/Ni–N–C SACs electrocatalyst toward CO2RR and rationally optimizing the electrolyte, an effective aqueous-phase Mg–CO2 battery is demonstrated to generate not only electricity, but also syngas with CO from the CO2RR and H2 from the chemical oxidation of Mg, together with higher-valued MgHPO4 phosphate. Notably, the output of electricity, the proportion of CO/H2 in syngas, and the yields/crystalline quality of MgHPO4 can be well regulated by manipulating the operation parameters. The Mg–CO2 battery generates a favorable open-circuit voltage of 1.44 V with a peak power density of 2.91 mW cm–2. Under the optimal condition, the Ni NPs/Ni–N–C SACs catalyst displays both a high FECO of 98.12% at −0.573 VRHE and a high CO2-to-CO current of −20.73 mA cm–2 at −0.973 VRHE, owing to the synergistic effect between Ni particles and Ni–N moieties. The proposed Mg–CO2 battery provides an intriguing approach for CO2 conversion and utilization in off-grid, with the advantage of coproduction of higher-valued chemicals at both electrodes.
A key consensus of implementing large-scale water splitting is developing highly efficient, durable, and earth-abundant electrocatalysts for oxygen evolution reaction (OER). In recent years, the Fe-based materials used in OER have attracted researchers' great attention around the globe, and Fe has been identified as the OER active sites. In this study, we firstly synthesized the coral-like FeSe/FeSe 2 heterostructure catalyst via a one-pot solvothermal method. We demonstrated that different components of FeSe/FeSe 2 heterostructure can facilitate the electron transfer process of the system, where a high Fe charge state promotes OER performance, rendering the coral-like FeSe/FeSe 2 heterostructure to be more promising Fe-based electrocatalyst for oxygen evolution reaction in alkaline. As expected, the asprepared FeSe/FeSe 2 heterostructure with highly charged iron and negatively charged selenium species exhibited better OER performance and needed only an overpotential of 309 mV to achieve an anodic current density of 10 mA cm À 2 . In addition, the catalyst had quick kinetics and good durability in alkaline medium. The present study would open up a potential avenue for the development of highly active non-noble-metal electrocatalysts.
Heterostructured oxides with versatile active sites, as a class of efficient catalysts for CO2 electrochemical reduction (CO2ER), are prone to undergo structure reconstruction under working conditions, thus bringing challenges to understanding the reaction mechanism and rationally designing catalysts. Herein, we for the first time elucidate the structural reconstruction of CuO/SnO2 under electrochemical potentials and reveal the intrinsic relationship between CO2ER product selectivity and the in‐situ evolved heterostructures. At ‐0.85 VRHE, the CuO/SnO2 evolves to Cu2O/SnO2 with high selectivity to HCOOH (Faradaic efficiency of 54.81%). Mostly interestingly, it is reconstructed to Cu/SnO2‐x at ‐1.05 VRHE with significantly improved Faradaic efficiency to ethanol of 39.8%. In‐situ Raman spectra and density functional theory (DFT) calculations reveal that the synergetic absorption of *COOH and *CHOCO intermediates at the interface of Cu/SnO2‐x favors the formation of *CO and decreases the energy barrier of C‐C coupling, leading to high selectivity to ethanol.
CO 2 utilization is one of the hottest research topics worldwide. As a class of newly emerging and promising catalysts for electrochemical CO 2 reduction (ECR) reaction, heteroatom-doped metal-N x -C single atom catalysts (M-N x -C SACs) attract extensive attentions. Nowadays, great progress, including structure modulation, identification of local coordination environment and ECR mechanism via advanced synthetic strategies, characterization techniques and theoretical calculations, have been achieved over heteroatom doped asymmetric M-N x -C SACs, which boost the ECR performances and deepen the understanding of ECR mechanism. In this context, we summarize recent progresses in heteroatomdoped asymmetric M-N x -C SACs, with emphasis on synthetic strategies and their applications in ECR reaction, along with current understanding on the ECR mechanisms both experimentally and theoretically. Finally, the challenges and perspectives for the heteroatom-doped asymmetric M-N x -C SACs towards ECR are proposed.
Heterostructured oxides with versatile active sites, as a class of efficient catalysts for CO2 electrochemical reduction (CO2ER), are prone to undergo structure reconstruction under working conditions, thus bringing challenges to understanding the reaction mechanism and rationally designing catalysts. Herein, we for the first time elucidate the structural reconstruction of CuO/SnO2 under electrochemical potentials and reveal the intrinsic relationship between CO2ER product selectivity and the in‐situ evolved heterostructures. At ‐0.85 VRHE, the CuO/SnO2 evolves to Cu2O/SnO2 with high selectivity to HCOOH (Faradaic efficiency of 54.81%). Mostly interestingly, it is reconstructed to Cu/SnO2‐x at ‐1.05 VRHE with significantly improved Faradaic efficiency to ethanol of 39.8%. In‐situ Raman spectra and density functional theory (DFT) calculations reveal that the synergetic absorption of *COOH and *CHOCO intermediates at the interface of Cu/SnO2‐x favors the formation of *CO and decreases the energy barrier of C‐C coupling, leading to high selectivity to ethanol.
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