The exploitation of highly efficient carbon dioxide reduction (CO 2 RR) electrocatalyst for methane (CH 4 ) electrosynthesis has attracted great attention for the intermittent renewable electricity storage but remains...
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The exploitation of highly efficient carbon dioxide reduction (CO 2 RR) electrocatalyst for methane (CH 4 ) electrosynthesis has attracted great attention for the intermittent renewable electricity storage but remains challenging. Here, N-heterocyclic carbene (NHC)-ligated copper single atom site (Cu SAS) embedded in metal–organic framework is reported (2Bn-Cu@UiO-67), which can achieve an outstanding Faradaic efficiency (FE) of 81 % for the CO 2 reduction to CH 4 at −1.5 V vs. RHE with a current density of 420 mA cm −2 . The CH 4 FE of our catalyst remains above 70 % within a wide potential range and achieves an unprecedented turnover frequency (TOF) of 16.3 s −1 . The σ donation of NHC enriches the surface electron density of Cu SAS and promotes the preferential adsorption of CHO* intermediates. The porosity of the catalyst facilitates the diffusion of CO 2 to 2Bn-Cu, significantly increasing the availability of each catalytic center.
Confinement of noble nanometals in a zeolite matrix is a promising way to special types of catalysts that show significant advantages in size control, site adjustment, and nano‐architecture design. The beauty of zeol...
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Confinement of noble nanometals in a zeolite matrix is a promising way to special types of catalysts that show significant advantages in size control, site adjustment, and nano‐architecture design. The beauty of zeolite‐confined noble metals lies in their unique confinement effects on a molecular scale, and thus enables spatially confined catalysis akin to enzyme catalysis. In this Minireview, the confined synthesis strategies of zeolite‐confined noble metals will be briefly discussed, showing the processes, advantages, features, and mechanisms. The confined catalysis carried on zeolite‐confined noble metals will be summarized, and great emphasis will be paid to the confinement effects involving size, encapsulation, recognition, and synergy. Great progress of atomic sites in the size effect, supercage stabilization in the encapsulation effect, site adsorption in the recognition effect, and cascade reaction in the synergy effect are highlighted. This Minireview is concluded with challenges and opportunities in terms of the synthesis of zeolite‐confined noble metals and their applications to design multifunctional catalysts with high catalytic activity, selectivity, and stability.
Developing large-scale monolithic perovskite/silicon tandem devices based on industrial Czochralski silicon wafers will likely have to adopt double-side textured architecture, given their optical benefits and low manu...
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Developing large-scale monolithic perovskite/silicon tandem devices based on industrial Czochralski silicon wafers will likely have to adopt double-side textured architecture, given their optical benefits and low manufacturing costs. However, the surface engineering strategies that are widely used in solution-processed perovskites to regulate the interface properties are not directly applicable to micrometric textures. Here, we devise a surface passivation strategy by dynamic spray coating (DSC) fluorinated thiophenethylammonium ligands, combining the advantages of providing conformal coverage and suppressing phase conversion on textured surfaces. From the viewpoint of molecular engineering, theoretical calculation and experimental results demonstrate that introducing trifluoromethyl group provide more effective surface passivation through strong interaction and energy alignment by forming a dipole layer. Consequently, the DSC treatment of this bifunctional molecule enables the tandem cells based on industrial silicon wafers to achieve a certified stabilized power conversion efficiency of 30.89 %. In addition, encapsulated devices display excellent operational stability by retaining over 97 % of their initial performance after 600 h continuous illumination.
The sodium dual ion battery (Na-DIB) technology is proposed as highly promising alternative over lithium-ion batteries for the stationary electrochemical energy-storage devices. However, the sluggish reaction kinetics...
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The sodium dual ion battery (Na-DIB) technology is proposed as highly promising alternative over lithium-ion batteries for the stationary electrochemical energy-storage devices. However, the sluggish reaction kinetics of anode materials seriously impedes their practical implementation. Herein, a Na-DIB based on TiSe 2 -graphite is reported. The high diffusion coefficient of Na-ions (3.21×10 −11 –1.20×10 −9 cm 2 s −1 ) and the very low Na-ion diffusion barrier (0.50 eV) lead to very fast electrode kinetics, alike in conventional surface capacitive storage systems. In-situ investigations reveal that the fast Na-ion diffusion involves four insertion stage compositions. A prototype cell shows a reversible capacity of 81.8 mAh g −1 at current density of 100 mA g −1 , excellent stability with 83.52 % capacity retention over 200 cycles and excellent rate performance, suggesting its potential for next-generation large scale high-performance stationary energy storage systems.
Biological ion channels penetrated through cell membrane form unique transport pathways for selective ionic conductance. Replicating the success of ion selectivity with mixed matrix membranes (MMMs) will enable new se...
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Biological ion channels penetrated through cell membrane form unique transport pathways for selective ionic conductance. Replicating the success of ion selectivity with mixed matrix membranes (MMMs) will enable new separation technologies but remains challenging. Herein, we report a soft substrate-assisted solution casting method to develop MMMs with penetrating subnanochannels for selective metal ion conduction. The MMMs are composed of penetrating Prussian white (PW) microcubes with subnanochannels in dense polyimide (PI) matrices, achieving selective monovalent metal ion conduction. The ion selectivity of K + /Mg 2+ is up to 14.0, and the ion conductance of K + can reach 45.5 μS with the testing diameter of 5 mm, which can be further improved by increasing the testing area. Given the diversity of nanoporous materials and polymer matrices, we expect that the MMMs with penetrating subnanochannels could be developed into a versatile nanofluidic platform for various emerging applications.
The corrosion, parasitic reactions, and aggravated dendrite growth severely restrict development of aqueous Zn metal batteries. Here, we report a novel strategy to break the hydrogen bond network between water molecul...
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The corrosion, parasitic reactions, and aggravated dendrite growth severely restrict development of aqueous Zn metal batteries. Here, we report a novel strategy to break the hydrogen bond network between water molecules and construct the Zn(TFSI) 2 -sulfolane-H 2 O deep eutectic solvents. This strategy cuts off the transfer of protons/hydroxides and inhibits the activity of H 2 O, as reflected in a much lower freezing point (<−80 °C), a significantly larger electrochemical stable window (>3 V), and suppressed evaporative water from electrolytes. Stable Zn plating/stripping for over 9600 h was obtained. Based on experimental characterizations and theoretical simulations, it has been proved that sulfolane can effectively regulate solvation shell and simultaneously build the multifunctional Zn-electrolyte interface. Moreover, the multi-layer homemade modular cell and 1.32 Ah pouch cell further confirm its prospect for practical application.
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