Search

Selective CO2 photoreduction to C2 hydrocarbons is significant but limited by the inadequate adsorption strength of the reaction intermediates and low efficiency of proton transfer. Herein, an ameliorative *CO adsorption and H2O activation strategy is realized via decorating bismuth oxychloride (BiOCl) nanostructures with different metal (Pt, Pd, and Au) species. Experimental and theoretical calculation results reveal that distinct *CO binding energies and *H acquisition abilities of the metal cocatalysts mediate the CO2 reduction activity and hydrocarbon selectivity. The relatively moderate *CO adsorption and *H supply over Pd/BiOCl endows it with the lowest free energy to generate *CHO, leading to its highest activity of hydrocarbon production. Specifically, the Pt cocatalyst can efficiently participate in H2O dissociation to deliver more *H for facilitating the protonation of the *CHO and *CHOH, thereby favoring CH4 production with 76.51% selectivity. A lower *H supply over Pd/BiOCl and Au/BiOCl results in a large energy barrier for *CHO or *CHOH protonation and thus a more thermodynamically favored OC─CHO coupling pathway, which endows them with vastly increased C2 hydrocarbon selectivity of 81.21% and 92.81%, respectively. The understanding of efficient C2 hydrocarbon production in this study sheds light on how materials can be engineered for photocatalytic CO2 reduction. [ABSTRACT FROM AUTHOR]

Two metal–organic frameworks (MOFs) with different Cu-centered coordination structures were synthesized. By introducing 4,4-bipyridine as a linker in the Cu-MOFs, we have discovered that Cu–O, instead of Cu–N, is the active site with higher electrocatalytical activity towards ascorbic acid, which is essential to understand and develop Cu-based ascorbic acid sensors. [ABSTRACT FROM AUTHOR]

Harvesting solar energy for efficient photothermal conversion and steam generation over solar evaporators is particularly significant in the context of comprehensive solar utilization toward solving the global shortage of fresh water. Herein, a flexible Ni-based metal–organic framework composite (NMC) with hierarchical structures is constructed as a photothermal material for solar steam-generation devices. Besides, a phase change material (PCM)-based thermal storage pack is incorporated into the solar evaporator to overcome the solar radiation intermittency. By virtue of the synergistic effect of the promising 3D structure and excellent water transport, the NMC-PCM evaporator possesses an outstanding evaporation performance (2.55 kg m−2 h−1) under 1 sun irradiation. More strikingly, owing to the enhanced light-to-heat performance as well as large heat storage capacity, the proposed evaporator achieves a high water-evaporation rate of 1.46 kg m−2 h−1 without sunlight irradiation. This work opens up opportunities to realize excellent energy capture for solar-driven clean water production and solar thermal storage not only under sunlight incidence but also in no light environment. [ABSTRACT FROM AUTHOR]

Eshelby tensors in elasticity are obtained for two-dimensional (2D) decagonal quasicrystal containing an ellipsoidal inclusion. Based on the intrinsic strain formula and Mori–Tanaka theory, the effective elastic properties of 2D decagonal composites are obtained. The effects of inclusion volume fraction and inclusion aspect ratio on elastic properties of composites with 2D decagonal quasicrystal are discussed. [ABSTRACT FROM AUTHOR]

Intermetallic compounds (IMCs) with fixed chemical composition and ordered crystallographic arrangement are highly desirable platforms for elucidating the precise correlation between structures and performances in catalysis. However, diffusing a metal atom into a lattice of another metal to form a controllably regular metal occupancy remains a huge challenge. Herein, we develop a general and tractable solvothermal method to synthesize the Bi-Pd IMCs family, including Bi2Pd, BiPd, Bi3Pd5, Bi2Pd5, Bi3Pd8 and BiPd3. By employing electrocatalytic CO2 reduction as a model reaction, we deeply elucidated the interplay between Bi-Pd IMCs and key intermediates. Specific surface atomic arrangements endow Bi-Pd IMCs different relative surface binding affinities and adsorption configuration for *OCHO, *COOH and *H intermediate, thus exhibiting substantially selective generation of formate (Bi2Pd), CO (BiPd3) and H2 (Bi2Pd5). This work provides a comprehensive understanding of the specific structure-performance correlation of IMCs, which serves as a valuable paradigm for precisely modulating catalyst material structures. Precise synthesis of Intermetallic compounds and understanding of the structure-performance correlation are highly desirable in catalysis. Here, the authors develop a general method to synthesize up to six BiPd intermetallic compounds and study the mechanism toward the electrocatalytic carbon dioxide reduction reaction. [ABSTRACT FROM AUTHOR]

An efficient electrocatalytic conversion of CO 2 into valuable multicarbon (C 2+ ) products requires enhanced C-C coupling of C1 intermediates. Herein, we combine a tandem effect with a confinement strategy to construct a hollow Cu 2 O@Ag nanoshell electrocatalyst with a well-defined porous structure to improve the *CO intermediate coverage on the catalyst surface. In CO 2 electroreduction, in situ Raman spectroscopy shows that the introduction of Ag can not only promote the CO intermediate production but also improve the stability of Cu + to capture the *CO intermediate due to a CO-tandem effect, and the fine-tuned hollowness degree and pore size of Cu 2 O@Ag create a spatially confined microenvironment for trapping CO 2 as well as the enrichment of CO, which greatly facilitate subsequent C-C coupling for C 2+ product. The optimized Cu 2 O@Ag-45 with a specific nanoconfinement exhibits an enhanced ethylene (C 2 H 4 ) production under the wide potential range from -0.4 to -1.2 V (vs RHE), and a Faradaic efficiency of 55.4% for C 2+ products could be achieved at -1.2 V (vs RHE). This study highlights a promising strategy for the electrochemical reduction of CO 2 to C 2+ products on efficient C-C coupling catalysts.

Selective CO 2 photoreduction to C 2 hydrocarbons is significant but limited by the inadequate adsorption strength of the reaction intermediates and low efficiency of proton transfer. Herein, an ameliorative *CO adsorption and H 2 O activation strategy is realized via decorating bismuth oxychloride (BiOCl) nanostructures with different metal (Pt, Pd, and Au) species. Experimental and theoretical calculation results reveal that distinct *CO binding energies and *H acquisition abilities of the metal cocatalysts mediate the CO 2 reduction activity and hydrocarbon selectivity. The relatively moderate *CO adsorption and *H supply over Pd/BiOCl endows it with the lowest free energy to generate *CHO, leading to its highest activity of hydrocarbon production. Specifically, the Pt cocatalyst can efficiently participate in H 2 O dissociation to deliver more *H for facilitating the protonation of the *CHO and *CHOH, thereby favoring CH 4 production with 76.51% selectivity. A lower *H supply over Pd/BiOCl and Au/BiOCl results in a large energy barrier for *CHO or *CHOH protonation and thus a more thermodynamically favored OC─CHO coupling pathway, which endows them with vastly increased C 2 hydrocarbon selectivity of 81.21% and 92.81%, respectively. The understanding of efficient C 2 hydrocarbon production in this study sheds light on how materials can be engineered for photocatalytic CO 2 reduction., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)