Luxiang Wang

The efficient photocatalytic production of hydrogen peroxide (H2O2) coupled with the selective reduction of carbon dioxide (CO2) to carbon monoxide (CO) represents a sustainable pathway for solar fuel synthesis and chemical production; however, it remains challenging due to inefficient charge separation and sluggish surface reaction kinetics. Although the two-dimensional (2D) sulfide In4SnS8 exhibits excellent visible-light absorption, its photocatalytic performance is fundamentally limited by rapid charge recombination. To address this limitation, a 2D/2D g-C3N4/In4SnS8 type-II heterojunction has been designed and constructed. This heterostructure achieves remarkable photocatalytic activity through the synergistic integration of interfacial engineering and a built-in electric field (IEF). The optimized g-C3N4/In4SnS8 heterojunction demonstrates production rates of 572 μmol L–1 h–1 for H2O2 and 425.1 μL g–1 h–1 for CO, significantly surpassing the performance of its individual components. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations reveal that *OOH serves as the key intermediate for H2O2 formation, while adsorbed *COOH is identified as a critical surface species during CO2 reduction. Furthermore, ultraviolet photoelectron spectroscopy (UPS) confirms that a spontaneously formed interfacial IEF is the primary driver for the directional separation and migration of photogenerated charges toward active sites. This work not only provides fundamental insights into the rational design of type-II heterojunction photocatalysts but also significantly expands their potential photocatalytic applications.

Electrocatalytic C–N coupling represents a green synthesis platform, yet the dynamic evolution of catalyst surfaces during the reaction remains poorly understood. Here, we report a nitrate‐dominated, preferential facet evolution on Cu single crystals that directs less active (110) and (100) facets toward the highly active (111) configuration. The Cu(111) surface delivers a urea yield of 5.2 mg h ⁻¹ cm ⁻² from CO ₂ and NO ₃ ⁻ , outperforming (110) and (100) by about 4‐ and 26‐fold, respectively, while maintaining excellent stability. Experimental and theoretical analyses reveal that this facet reconstruction is associated with spontaneous chemical interaction between nitrate and metallic copper, alongside the thermodynamic stability of the Cu(111) facet. Significantly, the pristine Cu(111) surface consistently outperforms Cu(110) and Cu(100), highlighting its intrinsic catalytic superiority. This work provides insights into nitrate‐dominated C–N coupling, advancing the design of dynamically active electrocatalysts.

Electrocatalytic C–N coupling represents a green synthesis platform, yet the dynamic evolution of catalyst surfaces during the reaction remains poorly understood. Here, we report a nitrate‐dominated, preferential facet evolution on Cu single crystals that directs less active (110) and (100) facets toward the highly active (111) configuration. The Cu(111) surface delivers a urea yield of 5.2 mg h ⁻¹ cm ⁻² from CO ₂ and NO ₃ ⁻ , outperforming (110) and (100) by about 4‐ and 26‐fold, respectively, while maintaining excellent stability. Experimental and theoretical analyses reveal that this facet reconstruction is associated with spontaneous chemical interaction between nitrate and metallic copper, alongside the thermodynamic stability of the Cu(111) facet. Significantly, the pristine Cu(111) surface consistently outperforms Cu(110) and Cu(100), highlighting its intrinsic catalytic superiority. This work provides insights into nitrate‐dominated C–N coupling, advancing the design of dynamically active electrocatalysts.

The strong intrinsic polarization field in two-dimensional CuInP2S6, stemming from the spontaneous polarization of its asymmetric Cu/In lattice, acts as an effective driver for charge separation and regulation. This, together with the synergistic interaction among its constituent multielement, substantially enhances the material's electrochemical activity, leading to fundamentally improved charge transport efficiency and high potential for sodium-ion storage. Herein, to further boost electrochemical performance, reduced graphene oxide (rGO) was introduced to fabricate a CuInP2S6/rGO composite. The composite exhibits remarkable sodium storage properties due to the combined effects of the intrinsic polarization field of CuInP2S6, the inherent multielement coupling, and efficient interfacial engineering with rGO. It maintains specific capacities of 459.5 (after 1700 cycles) and 398.5 mA h g-1 at high current densities of 5 and 20 A g-1, respectively. Density functional theory calculations reveal that incorporating rGO promotes Na+ adsorption and charge delocalization, weakens P–S bonds, and increases reactivity. This work confirms the feasibility of the polarized CuInP2S6/rGO composite for high-performance energy storage and clarifies its stepwise Na+ storage mechanism through ex/in situ analyses. It provides valuable insights for designing high-performance sodium-ion batteries electrodes by leveraging the intrinsic polarization and multielement synergy of functional materials.