Yiou Wang

Photocatalysis offers a promising route to sustainable energy, yet the role of carrier spin in charge transport and interfacial redox chemistry remains poorly understood. Chiral and magnetic catalysts selectively transmit spin‐compatible carriers, whereas non‐polarized light generates mixed‐spin populations, limiting carrier utilization. Herein, we demonstrate that circularly polarized light (CPL) reversibly modulates spin‐dependent carrier transport in Ni‐cocatalyst‐decorated, cysteine‐modified CdS nanorods, thereby promoting spin‐sensitive carrier utilization during aqueous methanol reforming. Optimized D(−)‐CdS/Ni exhibits a 71.1% higher hydrogen evolution rate under left‐handed CPL (LCP) than under right‐handed CPL (RCP) at identical light intensity and spectrum, achieving an apparent quantum efficiency of 74.4% at 420 nm while promoting methanol oxidation toward formic acid. CPL‐coupled magnetic conductive atomic force microscopy reveals that LCP increases the apparent spin polarization from 70.9% in the dark to 89.1%, whereas RCP suppresses it to 12.8%. Spin‐polarized calculations identify nonequivalent electronic channels, while spectroscopic and kinetic measurements support enhanced carrier extraction and reduced recombination under LCP. Together, these findings establish photon handedness as a reversible optical variable for modulating spin‐selective transport and photoredox chemistry, offering a strategy to complement material‐encoded spin filtering with dynamic optical control of carrier utilization.

Photocatalysis offers a promising route to sustainable energy, yet the role of carrier spin in charge transport and interfacial redox chemistry remains poorly understood. Chiral and magnetic catalysts selectively transmit spin‐compatible carriers, whereas non‐polarized light generates mixed‐spin populations, limiting carrier utilization. Herein, we demonstrate that circularly polarized light (CPL) reversibly modulates spin‐dependent carrier transport in Ni‐cocatalyst‐decorated, cysteine‐modified CdS nanorods, thereby promoting spin‐sensitive carrier utilization during aqueous methanol reforming. Optimized D(−)‐CdS/Ni exhibits a 71.1% higher hydrogen evolution rate under left‐handed CPL (LCP) than under right‐handed CPL (RCP) at identical light intensity and spectrum, achieving an apparent quantum efficiency of 74.4% at 420 nm while promoting methanol oxidation toward formic acid. CPL‐coupled magnetic conductive atomic force microscopy reveals that LCP increases the apparent spin polarization from 70.9% in the dark to 89.1%, whereas RCP suppresses it to 12.8%. Spin‐polarized calculations identify nonequivalent electronic channels, while spectroscopic and kinetic measurements support enhanced carrier extraction and reduced recombination under LCP. Together, these findings establish photon handedness as a reversible optical variable for modulating spin‐selective transport and photoredox chemistry, offering a strategy to complement material‐encoded spin filtering with dynamic optical control of carrier utilization.

Integrated carbon capture and utilization can reduce the energy penalty of CO ₂ valorization, but is often limited by slow transport between capture and catalytic sites. Here, we report a proximity‐engineered dual‐functional material for direct conversion of captured CO ₂ into syngas via isothermal calcium‐looping dry reforming of methane at 650°C. Embedding trace Ni into a CaO framework and introducing CeO ₂ creates abundant Ni–Ce–Ca interfacial sites with shortened carbonate diffusion pathways, enhanced oxygen mobility, and improved resistance to sintering and coking. The optimized material achieves a CO ₂ capture capacity of 12.6 mmol g ⁻¹ and a syngas yield of 58 mmol g ⁻¹ , representing up to a 2.9‐fold improvement over conventional materials. Operando spectroscopy and density functional theory reveal that captured carbonates are directly converted through a lower‐energy COOH‐mediated interfacial pathway, demonstrating an effective strategy to overcome transport limitations in integrated CO ₂ capture and conversion.

Water is essential in photosynthesis, acting both as a reactant and a medium regulating charge transport and reaction kinetics. While catalyst design has received significant attention, the impact of water structure on reactivity remains almost unexplored. Here, we report that water engineering via surfactant coacervates can significantly improve the performance of artificial photosynthesis for hydrogen production. By creating dynamic aqueous coacervate phases within a disrupted hydrogen-bond network, we create environments that yield more active, disordered water molecules. This tuned water state yields a stable hydrogen evolution rate of 918 mmol·g^-1·h^-1 and an apparent quantum efficiency of 69% at 420 nm in an aqueous methanol solution, demonstrating competitive catalytic performance. Spectroscopic and calorimetric characterizations, as well as computational simulations, indicate that surfactant coacervates increase the amount of intermediate water while weakening hydrogen bonding, thereby reducing the apparent activation energy, promoting charge transfer, and facilitating efficient catalysis. This study presents an approach to regulate water structure to enhance catalytic reactivity for solar hydrogen production, with broad potential for applications in water-involved catalytic systems.

The surficial active centers of photocatalysts play a critical role in photocatalytic reactions and require rational design to optimize their adsorption and activation properties for substrates. Single atoms anchored to metal oxide semiconductors, forming asymmetric oxygen-bridged dual-metal sites (M₁-O-M₂), exhibit tunable electronic properties for adsorption and activation. However, the catalytic mechanisms of each site remain unclear, and their full performance potential has yet to be explored. Herein, we report oxygen-bridged reductive V⁴⁺ and oxidative Cu^δ+ sites (Cu-O-V) for the photo-oxidative coupling of benzylamine (BA), enabled by the synthesis of single-atom Cu-anchored Na⁺ intercalated V₂O₅ (Cu-SA/NVO) nanoribbons. As characterized by electron paramagnetic resonance (EPR), X-ray absorption spectroscopy (XAS), and Raman spectroscopy, the introduction of Cu^δ+ sites increases the density of nearby V⁴⁺ sites, thereby facilitating the directional migration of photoelectrons to V sites and photoholes to Cu sites. The synergistic effect of the promoted charge transfer and oxygen-bridged dual sites achieved a yield of 2.73 mmol g^-1 h^-1 for photo-oxidative BA to NBI, which was nearly 3 times that of NVO and 91 times that of Cu-SA/V₂O₅ with a selectivity of up to 99%. In situ infrared spectroscopy detected a stronger stretching vibration of *Ph-CH═NH intermediate on Cu-SA/NVO, indicating the Cu-O-V structure facilitated the nucleophilic reaction of the BA intermediate. Density functional theory (DFT) results revealed that the Cu-O-V bridge significantly enhanced the adsorption of O₂ and BA, and lowered the reaction barrier for the conversion of *Ph-CH₂NH₂^•+ to *Ph-CH═NH, thereby substantially improving the yield of NBI. Our work provides new insights into the design and optimization of photocatalysts.

Precise optical control over catalytic pathways remains a major challenge in solar‐driven hydrogen production. Here, we report a reversible light‐handedness‐dependent switching mechanism between photocatalysis and photothermal catalysis using a standard Au@CdS nanocatalyst functionalized with chiral cysteine ligands. The switching behavior is governed by the interplay of chemical chirality and circularly polarized light, mediated by the chirality‐induced spin selectivity effect. When the handedness of circularly polarized light matches the catalyst's chirality, spin‐polarized carriers are efficiently transferred, favoring photocatalysis. In contrast, mismatched conditions suppress charge transfer, enhance recombination, and induce localized heating, shifting the reaction toward photothermal catalysis. Tuning the handedness of circularly polarized light to mismatch the catalyst chirality induces a significant photothermal effect, with temperatures reaching 343 K and hydrogen evolution rates of up to 4.8 mmol g ⁻¹ h ⁻¹ , doubling the performance in the matched case. This study introduces a light‐handedness‐controlled catalytic switch that enables dynamic modulation between two reaction modes using the same chiral catalyst, advancing our mechanistic understanding of spin‐dependent photothermal phenomena and establishing a versatile platform for optically tunable solar fuel production. The interaction of chemical and optical chirality offers a novel approach to designing next‐generation photocatalysts that can be tailored for energy conversion.

Precise optical control over catalytic pathways remains a major challenge in solar‐driven hydrogen production. Here, we report a reversible light‐handedness‐dependent switching mechanism between photocatalysis and photothermal catalysis using a standard Au@CdS nanocatalyst functionalized with chiral cysteine ligands. The switching behavior is governed by the interplay of chemical chirality and circularly polarized light, mediated by the chirality‐induced spin selectivity effect. When the handedness of circularly polarized light matches the catalyst's chirality, spin‐polarized carriers are efficiently transferred, favoring photocatalysis. In contrast, mismatched conditions suppress charge transfer, enhance recombination, and induce localized heating, shifting the reaction toward photothermal catalysis. Tuning the handedness of circularly polarized light to mismatch the catalyst chirality induces a significant photothermal effect, with temperatures reaching 343 K and hydrogen evolution rates of up to 4.8 mmol g ⁻¹ h ⁻¹ , doubling the performance in the matched case. This study introduces a light‐handedness‐controlled catalytic switch that enables dynamic modulation between two reaction modes using the same chiral catalyst, advancing our mechanistic understanding of spin‐dependent photothermal phenomena and establishing a versatile platform for optically tunable solar fuel production. The interaction of chemical and optical chirality offers a novel approach to designing next‐generation photocatalysts that can be tailored for energy conversion.

Plastic waste has caused severe global environmental pollution and health issues due to the high production rate and lack of proper disposal technology. Traditional methods to deal with plastic waste, such as incineration and landfilling, are deemed unsustainable and energy‐intensive. A promising alternative is the photocatalytic conversion of plastic waste, using sunlight as a sustainable and carbon‐neutral energy source to break down plastic waste under ambient pressure and low temperatures. This review aims to provide a comprehensive summary of recent advancements in plastic photoconversion, with an emphasis on the catalysts and reaction pathways. The mechanisms and reaction routes are first reviewed, followed by a detailed discussion of strategies to design catalysts for improved performance in photoconversion. Then, examples of photothermal degradation processes are presented. Finally, current strategies, challenges, and possible future directions of plastic photoconversion are summarized and discussed.

Selective catalytic reduction of nitrogen oxides with NH₃ at low temperatures remains a crucial goal for industrial applications. However, effective catalysts operating at 70–90 °C are rarely reported, limiting SCR scenarios to high‐temperature conditions. Herein, we report a unique MnO₂ nanofilament catalyst grown on activated semi‐coke synthesized via a one‐step in situ hydrothermal approach, which exhibits a stable and marked 100 % conversion rate of NO to N₂ with 100 % selectivity at 90 °C, superior to the other prepared structures (nanowires, nanorods, and nanotubes). Temperature‐programmed desorption shows a large number of acid sites on MnO₂(NFs)/ASC, benefiting the formation of NH₄⁺ ions. Meanwhile, diffuse reflectance infrared Fourier transform spectroscopy reveals the activation of NO with O₂ to form bidentate nitrate/bridging nitrate NO₂ intermediates via bidentate nitrate species, triggering the Fast SCR with NH₃ at low temperatures. Such an effective, easy‐to‐prepare, and low‐cost catalyst paves a new pathway for low‐temperature SCR for a wide range of application scenarios.