The rational design of a heterostructural photocatalysts with efficient charge separation and accelerated interfacial charge transfer holds great promise for boosting photocatalytic activity. Herein, we have developed a unique hierarchical In_4/3P₂S₆/TiO₂ heterojunction with P-O interfacial bonding for photocatalytic water reduction. By integrating emerging In_4/3P₂S₆ nanosheets through intense interfacial coupling effect, the optimized In_4/3P₂S₆/TiO₂ heterostructure exhibits a remarkably enhanced photocatalytic H₂ evolution activity compared to that of pristine TiO₂. Combined experimental and theoretical results confirm that multiple interfacial bonded S-scheme charge transfer pathways are established in the In_4/3P₂S₆/TiO₂ photocatalyst, which synergistically promote charge separation and transfer through the robust interfacial electric field and rapid charge migration pathways formed by interfacial bonds. This study emphasizes the significance of developing novel interfacial bonded In_4/3P₂S₆-based S-scheme heterostructures, paving a new strategy towards enhancing photocatalytic activity for H₂ evolution.

Heterogeneous advanced oxidation processes (AOPs) based on non-radical reactive species are considered as a powerful technology for wastewater purification due to their long half-lives and high adaptation in a wide pH range. Herein, we fabricate surface Co defect-rich spinel ZnCo₂O₄ porous nanosheets, which can generate ≡Co^IV=O and ¹O₂ over a wide pH range of 3.81–10.96 by the formation of amphoteric ≡Zn(OH)₂ in peroxymonosulfate (PMS) activation process. Density functional theory (DFT) calculations show Co defect-rich ZnCo₂O₄ possesses much stronger adsorption ability and more electron transfer to PMS. Moreover, the adsorption mode changes from terminal oxygen Co–O–Co to Co–O, accelerating the polarization of adjacent oxygen, which is beneficial to the generation of ≡Co^IV=O and ¹O₂. Co defect-rich ZnCo₂O₄ porous nanosheets exhibit highly active PMS activation activity and stability in p-nitrophenol (PNP) degradation, whose toxicity of degradation intermediates is significant reduction. The Co defect-rich ZnCo₂O₄ nanosheet catalyst sponge/PMS system achieved stable and efficient removal of PNP with a removal efficiency higher than 93% over 10 h. This work highlights the development of functional catalyst and provides an atomic-level understanding into non-radical PMS activation process in wastewater treatment.

Electrocatalytic reduction of CO₂ into high energy-density fuels and value-added chemicals under mild conditions can promote the sustainable cycle of carbon and decrease current energy and environmental problems. Constructing electrocatalyst with high activity, selectivity, stability, and low cost is really matter to realize industrial application of electrocatalytic CO₂ reduction (ECR). Metal–nitrogen–carbon (M–N–C), especially Ni–N–C, display excellent performance, such as nearly 100% CO selectivity, high current density, outstanding tolerance, etc., which is considered to possess broad application prospects. Based on the current research status, starting from the mechanism of ECR and the existence form of Ni active species, the latest research progress of Ni–N–C electrocatalysts in CO₂ electroreduction is systematically summarized. An overview is emphatically interpreted on the regulatory strategies for activity optimization over Ni–N–C, including N coordination modulation, vacancy defects construction, morphology design, surface modification, heteroatom activation, and bimetallic cooperation. Finally, some urgent problems and future prospects on designing Ni–N–C catalysts for ECR are discussed. This review aims to provide the guidance for the design and development of Ni–N–C catalysts with practical application.