Integrating H₂O₂ evolution with oxidative organic synthesis in a semiconductor-driven photoredox reaction is highly attractive since H₂O₂ and high-value chemicals can be concurrently produced using solar light as the only energy input. The dual-functional photocatalytic approach, free from sacrificial agents, enables simultaneous production of H₂O₂ and high-value organic chemicals. This strategy promises a green and sustainable organic synthesis with minimal greenhouse gas emissions. In this review, we first elucidate the fundamental principles of cooperative photoredox integration of H₂O₂ synthesis and selective organic oxidation with simultaneous utilization of photoexcited electrons and holes over semiconductor-based photocatalysts. Afterwards, a thorough review on the recent advancements of cooperative photoredox synthesis of H₂O₂ and value-added chemicals is presented. Notably, in-depth discussions and insights into the techniques for unravelling the photoredox reaction mechanisms are elucidated. Finally, critical challenges and prospects in this thriving field are comprehensively discussed. It is envisioned that this review will serve as a pivotal guidance on the rational design of such dual-functional photocatalytic system, thereby further stimulating the development of economical and environmentally benign H₂O₂ and high-value chemicals production.

The interrelated side reactions and dendrites growth severely destabilize the electrode/electrolyte interfaces, resulting in the difficult application of aqueous Zn ion batteries (AZIBs). Hydrophobic protective layer possesses natural inhibition ability for side reactions. However, the conventional protective layer with plane structure is difficult to attain joint regulation of side reaction and Zn nucleation. Herein, a novel three-dimensional (3D) electrically conductive and hydrophobic (3DECH) interface is elaborated to enable stable Zn anode. The as-prepared 3DECH interface presents a uniform 3D morphology with hydrophobic property, large specific surface area, abundant zincophilic sites, and excellent electroconductivity. Therefore, the 3DECH interface achieves uniform nucleation and dendrite-free deposition from synergetic benefits: (1) increased nucleation sites and reduced local current density through the special 3D structure and (2) uniform electric potential distribution and rapid Zn²⁺ transport due to the electroconductive alloy chemistry, thus coupling the hydrophobic property to obtain a highly reversible Zn anode. Consequently, the modified anode achieves a superior coulombic efficiency of 99.88% over 3500 cycles, and the pouch cells using modified anode and LiMn₂O₄ (LMO) cathode retain a capacity of 84 mAh g⁻¹ after 700 cycles at a reasonable depth discharge of 36%, without dendrite piercing and “dead Zn.”

The development of highly efficient sodium-ion batteries depends critically on the successful exploitation of advanced anode hosts that is capable of overcoming sluggish reaction kinetics while also withstanding severe structural deformation triggered by the large radius of Na⁺-insertion. Herein, a hierarchically hybrid material with hetero-Co₃S₄/NiS hollow nanosphere packaged into a densified N-doped carbon matrix (Co₃S₄/NiS@N-C) was designed and fabricated utilizing CoNi-glycerate as the self-sacrifice template, making the utmost of the synergistic effect of hetero-Co₃S₄/NiS with strong electric field and rich reaction active-sites together with the densified outer-carbon scaffolds with remarkable electronic conductivity and robust mechanical toughness. As anticipated, as-fabricated Co₃S₄/NiS@N-C anode affords remarkable specific capacity, prolonged cycle lifespan up to 2 400 cycles with an only 0.05% fading each cycle at 20.0 A g⁻¹, and excellent rate feature (354.9 mAh g⁻¹ at 30.0 A g⁻¹), one of the best performances for most existing Co₃S₄/NiS-based anodes. Ex situ structural characterizations in tandem with theoretical analysis demonstrate the reversible insertion-conversion mechanism of initially proceeding with Na⁺ de-/intercalation and superior heterogeneous interfacial reaction behavior with strong Na⁺-adsorption ability. Further, sodium-ion full cell and hybrid capacitor based on Co₃S₄/NiS@N-C anode exhibit impressive electrochemical characteristics on cycling performance and rate capability, showcasing its outstanding feasibility toward practical use.

Although zinc-air batteries (ZABs) are regarded as one of the most prospective energy storage devices, their practical application has been restricted by poor air electrode performance. Herein, we developed a free-standing air electrode that is fabricated on the basis of a multifunctional three-dimensional interconnected graphene network. Specifically, a three-dimensional interconnected graphene network with fast mass and electron transport ability, prepared by catalyzing growth of graphene foam on nickel foam and then filling reduced graphene oxide into the pores of graphene foam, is used to anchor iron phthalocyanine molecules with atomic Fe-N₄ sites for boosting the oxygen reduction during discharging and nanosized FeNi hydroxides for accelerating the oxygen evolution during charging. As a result, the obtained air electrode exhibited an ultra-small electrocatalytic overpotential of 0.603 V for oxygen reactions, a high peak power density of 220.2 mW cm^-2, and a small and stable charge-discharge voltage gap of 0.70 V at 10 mA cm^-2 after 1136 cycles. Furthermore, in situ Raman spectroscopy together with theoretical calculations confirmed that phase transformation of FeNi hydroxides takes place from α-Ni(OH)_x to β-Ni(OH)_x to γ-Ni^(3+δ)+OOH for the oxygen evolution reaction and Ni is the active center while Fe enhances the activity of Ni active sites.

Although MXene has attracted great interest in diverse fields, it is susceptible to oxidation in water (H₂O) with transition metal ions such as Co²⁺, Fe²⁺, and Cu²⁺, which is pronounced at high temperatures. This impedes the preparation of MXene-based composites and their functional applications. Here, this study revealed that Co²⁺ increases the maximum and average atomic charge of H in H₂O to improve the reactivity of H₂O, which leads to the fact that Co²⁺ catalyzes the oxidation of Ti₃C₂T_x MXene. Furthermore, the addition of N,N-dimethyl formamide (DMF) reduces the H₂O activity and improves the oxidation stability of Ti₃C₂T_x in the presence of Co²⁺ via preferentially forming coordination bonds with Co²⁺. This strategy is also effective in enhancing the oxidation tolerance of Ti₃C₂T_x to Fe²⁺ in H₂O. Moreover, it is feasible to enhance the oxidation stability of Ti₂CT_x MXene in H₂O with the existence of Co²⁺. By virtue of these, the CoO/Ti₃C₂T_x composite was successfully prepared without obvious Ti₃C₂T_x oxidation, which is desirable to harness the advantages of Ti₃C₂T_x as the complementary component for lithium-ion batteries. This work provides a straightforward paradigm to enhance the oxidation resistance of MXene in H₂O in the presence of transition metal ions and at high temperatures, which opens a new vista to use MXene for target applications.

Side-chain symmetry-breaking strategy plays an important role in developing photovoltaic materials for high-efficiency all-small-molecule organic solar cells (ASM OSCs). However, the power conversion efficiencies (PCEs) of ASM OSCs still lag behind their polymer-based counterparts, which can be attributed to the difficulties in achieving favorable morphology. Herein, two asymmetric porphyrin-based donors named DAPor-DPP and DDPor-DPP were synthesized, presenting stronger intermolecular interaction and closer molecular stacking compared to the symmetric ZnP-TEH. The DAPor-DPP:6TIC blend afforded a favorable morphology with nanoscale phase separation and more ordered molecular packing, thus achieving more efficient charge transportation and suppressed charge recombination. Consequently, the DAPor-DPP:6TIC-based device exhibited superior photovoltaic parameters, yielding a champion PCE of 16.62% higher than that of the DDPor-DPP-based device (14.96%). To our knowledge, 16.62% can be ranked as one of the highest PCE values among the binary ASM OSC filed. This work provides a prospective approach to address the challenge of ASM OSCs in improving film morphology and further achieving high efficiency via side-chain symmetry-breaking strategy, exhibiting great potential in constructing efficient ASM OSCs.

Spider silk, possessing exceptional combination properties, is classified as a bio-gel fiber. Thereby, it serves as a valuable origin of inspiration for the advancement of various artificial gel fiber materials with distinct functionalities. Gel fibers exhibit promising potential for utilization in diverse fields, including smart textiles, artificial muscle, tissue engineering, and strain sensing. However, there are still numerous challenges in improving the performance and functionalizing applications of spider silk-inspired artificial gel fibers. Thus, to gain a penetrating insight into bioinspired artificial gel fibers, this review provided a comprehensive overview encompassing three key aspects: the fundamental design concepts and implementing strategies of gel fibers, the properties and strengthening strategies of gel fibers, and the functionalities and application prospects of gel fibers. In particular, multiple strengthening and toughening mechanisms were introduced at micro, nano, and molecular-level structures of gel fibers. Additionally, the existing challenges of gel fibers are summarized. This review aims to offer significant guidance for the development and application of artificial gel fibers and inspire further research in the field of high-performance gel fibers.

Nanotechnology-inspired small-sized water-enabled electricity generation (WEG) has sparked widespread research interest, especially when applied as an electricity source for off-grid low-power electronic equipment and systems. Currently, WEG encompasses a wide range of physical phenomena, generator structures, and power generation environments. However, a systematic framework to clearly describe the connections and differences between these technologies is unavailable. In this review, a comprehensive overview of generator technologies and the typical mechanisms for harvesting water energy is provided. Considering the different roles of water in WEG processes, the related technologies are presented as two different scenarios. Moreover, a detailed analysis of the electrical potential formation in each WEG process is presented, and their similarities and differences are elucidated. Furthermore, a comprehensive compilation of advanced generator architectures and system designs based on hydrological cycle processes is presented, along with their respective energy efficiencies. These nanotechnology-inspired small-sized WEG devices show considerable potential for applications in the Internet of Things ecosystem (i.e., microelectronic devices, integrated circuits, and smart clothing). Finally, the prospects and future challenges of WEG devices are also summarized.

Precisely tuning bicomponent intimacy during reactions by traditional methods remains a formidable challenge in the fabrication of highly active and stable catalysts because of the difficulty in constructing well-defined catalytic systems and the occurrence of agglomeration during assembly. To overcome these limitations, a PtRuPNiO@TiO_x catalyst on a Ti plate was prepared by ultrasound-assisted low-voltage plasma electrolysis. This method involves the oxidation of pure Ti metal and co-reduction of strong metals at 3000°C, followed by sonochemical ultrasonication under ambient conditions in an aqueous solution. The intimacy of the bimetals in PtRuPNiO@TiO_x is tuned, and the metal nanoparticles are uniformly distributed on the porous titania coating via strong metal-support interactions by leveraging the instantaneous high-energy input from the plasma discharge and ultrasonic irradiation. The intimacy of PtRuPNiO@TiO_x increases the electron density on the Pt surface. Consequently, the paired sites exhibit a high hydrogen evolution reaction activity (an overpotential of 220 mV at a current density of 10 mA cm⁻² and Tafel slope of 186 mV dec⁻¹), excellent activity in the hydrogenation of 4-nitrophenol with a robust stability for up to 20 cycles, and the ability to contrast stated catalysts without ultrasonication and plasma electrolysis. This study facilitates industrially important reactions through synergistic chemical interactions.

Highly crystalline organic semiconductors are ideal materials for photocatalytic hydrogen evolution in water splitting. However, the instability and complex synthesis processes of most reported organic molecule-based photocatalysts restrict their applications. In this study, we introduce benzo [1,2-b:4,5-bʹ] bis [1] benzothiophene-3,9-dicarboxylic acid, 5,5,11,11-tetraoxide (FSOCA), a highly crystalline, stable molecular crystal that is easy to synthesize and serves as an efficient photocatalyst for the hydrogen evolution reaction. FSOCA exhibits high efficiency in sacrificial hydrogen evolution reaction (760 µmol h⁻¹, 76 mmol g⁻¹ h⁻¹ at 330 mW cm⁻²; 570 µmol h⁻¹, 57 mmol g⁻¹ h⁻¹ at 250 mW cm⁻²), and FSOCA remains stable during photocatalysis for up to 400 h. Experiments and theoretical studies confirmed the presence of hydrogen bonds between the sulfone group and the sacrificial agent (ascorbic acid). This interaction significantly improved the oxidation reaction kinetics and boosted the photocatalytic performance. This study presents a scalable and convenient approach to synthesize highly crystalline, active, and stable organic photocatalysts with potential applications in large-scale photocatalysis.