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Electrocatalytic CO2 reduction (ECR) powered by renewable electricity has attracted of wide attention because of its advantages to produce high‐value‐added chemicals and fuels. Additionally, ECR played a crucial role in addressing the challenge of excessive fossil fuel consumption caused by global warming. Herein, a unique armor structure with Ni nanoparticles coated by a carbon shell containing Ni─N─C (Ni─NP@Ni─SA) for industrial ECR to CO in pH‐universal electrolytes is designed. Ni─NP@Ni─SA catalyst exhibits ≈100% CO Faradaic efficiency, and CO partial current density can reach 500, 361, and 615 mA cm−2 in strong alkaline (pH 14), neutral (pH 7.2) and strong acidic (pH 1) electrolytes, respectively. Moreover, Ni─NP@Ni─SA can drive the rechargeable Zn‐CO2 battery with a high power density of 3.45 mW cm−2, and outstanding stability over 36 h. The structural characterizations and theoretical calculation together present that the electron penetration effect of Ni─NP@Ni─SA can strengthen the electronic enrichment state of Ni single atom, which facilitates the reaction kinetics of ECR by decreasing the formation energy barrier of key intermediate *COOH. This work pioneers a new design strategy to enhance the activity of single‐atom catalysts and seek high‐efficiency electrocatalysts for ECR in pH‐universal electrolytes. [ABSTRACT FROM AUTHOR]

Developing robust electrocatalysts and advanced devices is important for electrochemical carbon dioxide (CO2) reduction toward the generation of valuable chemicals. We present herein a carbon‐confined indium oxide electrocatalyst for stable and efficient CO2 reduction. The reductive corrosion of oxidative indium to the metallic state during electrolysis could be prevented by carbon protection, and the applied carbon layer also optimizes the reaction intermediate adsorption, which enables both high selectivity and activity for CO2 reduction. In a liquid‐phase flow cell, the formate selectivity exceeds 90 % in a wide potential window from −0.8 V to −1.3 V vs. RHE. The continuous production of ca. 0.12 M pure formic acid solution is further demonstrated at a current density of 30 mA cm−2 in a solid‐state electrolyte mediated reactor. This work provides significant concepts in the parallel development of electrocatalysts and devices for carbon‐neutral technologies. [ABSTRACT FROM AUTHOR]

Bimetallic sulfides are expected to realize efficient CO2 electroreduction into formate over a wide potential window, however, they will undergo in situ structural evolution under the reaction conditions. Therefore, clarifying the structural evolution process, the real active site and the catalytic mechanism is significant. Here, taking Cu2SnS3 as an example, we unveiled that Cu2SnS3 occurred self‐adapted phase separation toward forming the stable SnO2@CuS and SnO2@Cu2O heterojunction during the electrochemical process. Calculations illustrated that the strongly coupled interfaces as real active sites driven the electron self‐flow from Sn4+ to Cu+, thereby promoting the delocalized Sn sites to combine HCOO* with H*. Cu2SnS3 nanosheets achieve over 83.4 % formate selectivity in a wide potential range from −0.6 V to −1.1 V. Our findings provide insight into the structural evolution process and performance‐enhanced origin of ternary sulfides under the CO2 electroreduction. [ABSTRACT FROM AUTHOR]

We report an amino‐functionalized indium‐organic framework for efficient CO2 reduction to formate. The immobilized amino groups strengthen the absorption and activation of CO2 and stabilize the active intermediates, which endow an enhanced catalytic conversion to formate despite the inevitable reduction and reconstruction of the functionalized indium‐based catalyst during electrocatalysis. The reconstructed amino‐functionalized indium‐based catalyst demonstrates a high Faradaic efficiency of 94.4 % and a partial current density of 108 mA cm−2 at −1.1 V vs. RHE in a liquid‐phase flow cell, and also delivers an enhanced current density of ca. 800 mA cm−2 at 3.4 V for the formate production in a gas‐phase flow cell configuration. This work not only provides a molecular functionalization and assembling concept of hybrid electrocatalysts but also offers valuable understandings in electrocatalyst evolution and reactor optimization for CO2 electrocatalysis and beyond. [ABSTRACT FROM AUTHOR]

Supercapacitors possess important prospects in power supply, owing to the characteristics of fast charging/discharging and long cycling life. As emerging materials, metal‐organic frameworks (MOFs) are the cutting‐edge electrode active materials for supercapacitors due to their good conductivity, tunable pore structure, as well as diverse composition. In this Minireview, we summarize the recent progress in MOF electrodes for supercapacitors. We focus on the synthesis of intrinsically conductive MOFs constructed from different organic linkers and adjustable metal ions, and the preparation of conductive MOF composites hybridized with conducting materials (conducting polymers and carbons). Following the discussion of both different types of conductive MOFs and their composites in supercapacitors, the challenges, and opportunities of conductive MOF electrodes for supercapacitors are further prospected at the end of this contribution, which would provide some valuable insights in facilitating the use of MOF materials in energy‐storage applications. [ABSTRACT FROM AUTHOR]

As a way to drive chemical reactions by renewable solar energy, photocatalytic technology is an appealing strategy for carbon recycle and value‐added CO2 utilization mimicking the natural photosynthetic system to remedy energy and environmental problems. During the recent decades of exploration, extensive research has been reported on 2D nanomaterials in photocatalytic CO2 reduction because of their unique structural properties. This review highlights the ongoing development of modification strategies for 2D nanomaterials from the viewpoints of defect engineering, surface modification, and hybrid construction, following the sequence of inside‐to‐outside design of the photocatalysts. These methodologies can expand the scope of light absorption, promote the separation of photogenerated charge carriers, and enhance the adsorption and activation of CO2, thus effectively improve the photocatalytic efficiency. The future challenges and opportunities for developing modified 2D photocatalysts are also discussed. It is hoped that this review can provide useful guidelines toward further research on 2D nanocatalysis for CO2 photocatalytic conversion. [ABSTRACT FROM AUTHOR]

Electrocatalytic conversion of carbon dioxide (CO2) is promising for balancing carbon cycles while producing value‐added feedstocks. Herein, ultrathin ZnIn2S4 nanosheets with abundant Zn vacancies are demonstrated for electrochemically reducing CO2 to formate. Specifically, a partial current density of 245 mA cm−2 with a near‐unity faradaic efficiency of 94 % for formate generation was achieved over the ultrathin ZnIn2S4 nanosheets in a flow cell configuration. Experimental and theoretical results revealed that abundant Zn vacancies in the ultrathin ZnIn2S4 nanosheets with a high electrochemically active surface area synergistically optimized the intermediate binding energy and contributed to the boosted selectivity and activity. This work may provide useful understandings in designing efficient catalysts for selective CO2 electroreduction. [ABSTRACT FROM AUTHOR]

Carbon dioxide (CO2) conversion is promising in alleviating the excessive CO2 level and simultaneously producing valuables. This work reports the preparation of carbon nanorods encapsulated bismuth oxides for the efficient CO2 electroconversion toward formate production. This resultant catalyst exhibits a small onset potential of −0.28 V vs. RHE and partial current density of over 200 mA cm−2 with a stable and high Faradaic efficiency of 93 % for formate generation in a flow cell configuration. Electrochemical results demonstrate the synergistic effect in the Bi2O3@C promotes the rapid and selective CO2 reduction in which the Bi2O3 is beneficial for improving the reaction kinetics and formate selectivity, while the carbon matrix would be helpful for enhancing the activity and current density of formate production. This work provides effective bismuth‐based MOF derivatives for efficient formate production and offers insights in promoting practical CO2 conversion technology. [ABSTRACT FROM AUTHOR]