Xing Huang

The strong metal–support interaction (SMSI) has traditionally been viewed as a static phenomenon that modulates catalysis through site blocking. Here, we challenge this classical view by demonstrating that SMSI in Au/ZnO is an atmosphere‐dependent dynamic process that can be harnessed to engineer catalytic interfaces. Using in situ transmission electron microscopy, infrared spectroscopy, and X‐ray photoelectron spectroscopy, we track the structural evolution of the Au/ZnO interface throughout redox cycles and reaction conditions. Under H ₂ , oxygen vacancy formation triggers ZnO _x encapsulation, followed by AuZn alloying at elevated temperature, which induces nanoparticle reconstruction and expands the metal‐support interfacial area. Upon exposure to O ₂ , the alloy decomposes, and the ZnO _x overlayer dewets into nanoislands, with some regions undergoing complete retraction. Under CO oxidation conditions, the fully encapsulated state is lost, yet the H ₂ ‐pretreated catalyst exhibits superior activity and stability. This enhancement arises from alloying‐induced interface reconstruction together with residual ZnO nanoislands that persist after dewetting, creating an enlarged and highly active metal–oxide interface. Our work demonstrates a transient‐overlayer strategy for catalyst design, in which a pre‐formed SMSI layer serves as a precursor that, through controlled redox cycling or reaction conditions, transforms into a high‐interface area, sintering‐resistant catalytic architecture, thereby transcending the classical encapsulation‐activity dilemma.

The strong metal–support interaction (SMSI) has traditionally been viewed as a static phenomenon that modulates catalysis through site blocking. Here, we challenge this classical view by demonstrating that SMSI in Au/ZnO is an atmosphere‐dependent dynamic process that can be harnessed to engineer catalytic interfaces. Using in situ transmission electron microscopy, infrared spectroscopy, and X‐ray photoelectron spectroscopy, we track the structural evolution of the Au/ZnO interface throughout redox cycles and reaction conditions. Under H ₂ , oxygen vacancy formation triggers ZnO _x encapsulation, followed by AuZn alloying at elevated temperature, which induces nanoparticle reconstruction and expands the metal‐support interfacial area. Upon exposure to O ₂ , the alloy decomposes, and the ZnO _x overlayer dewets into nanoislands, with some regions undergoing complete retraction. Under CO oxidation conditions, the fully encapsulated state is lost, yet the H ₂ ‐pretreated catalyst exhibits superior activity and stability. This enhancement arises from alloying‐induced interface reconstruction together with residual ZnO nanoislands that persist after dewetting, creating an enlarged and highly active metal–oxide interface. Our work demonstrates a transient‐overlayer strategy for catalyst design, in which a pre‐formed SMSI layer serves as a precursor that, through controlled redox cycling or reaction conditions, transforms into a high‐interface area, sintering‐resistant catalytic architecture, thereby transcending the classical encapsulation‐activity dilemma.

The dehydroaromatization of ethane to aromatics is a highly attractive yet challenging route for valorizing the second‐most abundant component of natural gas. Here, we report bimetallic xGa0.8Pt/HZSM‐5 catalysts that exhibit markedly enhanced stability and coke resistance compared to their monometallic counterparts. The optimal 0.5Ga0.8Pt/HZSM‐5 catalyst affords an initial ethane conversion of 52% and an aromatics space–time yield of 5.4 mmol _arom ·g _cat ⁻¹ ·h ⁻¹ , with an exceptionally low deactivation rate constant of 0.007 h ⁻¹ over 10 h. An optimal Ga/Pt ratio fosters a strong synergistic effect, as evidenced by gas adsorption–desorption and in situ spectroscopic studies. Crucially, active site characterization reveals that the GaPt alloy formed in this catalyst works in concert with the acid sites of HZSM‐5, enhancing both dehydrogenation and aromatization while simultaneously suppressing coke formation. These findings provide direct evidence for the promotional role of bimetallic alloy sites and offer a rational strategy for designing stable Pt‐based catalysts for light alkane dehydroaromatization.

Ti‐MWW is an important member of Ti‐containing zeolites, industrially employed as heterogeneous catalyst for selective oxidations. However, the development of more active variants is often hampered by the lack of characterization methods able to track transformations and interplay between a multitude of species; this is further exacerbated by the use of post‐synthetic modifications. Combining microscopy and various spectroscopic techniques show that the promotional role of Zn is closely linked to its healing of hydrophilic silanol nests, while simultaneously generating small TiO _x clusters. Notably, these changes are accompanied by Ti weight loading dependent modifications of the extra‐framework TiO ₂ and formation of Zn species. Overall, our study not only highlights the interplay between a plethora of species, but enables a more rational development of post‐modification of Ti‐containing zeolites.

Ti‐MWW is an important member of Ti‐containing zeolites, industrially employed as heterogeneous catalyst for selective oxidations. However, the development of more active variants is often hampered by the lack of characterization methods able to track transformations and interplay between a multitude of species; this is further exacerbated by the use of post‐synthetic modifications. Combining microscopy and various spectroscopic techniques show that the promotional role of Zn is closely linked to its healing of hydrophilic silanol nests, while simultaneously generating small TiO _x clusters. Notably, these changes are accompanied by Ti weight loading dependent modifications of the extra‐framework TiO ₂ and formation of Zn species. Overall, our study not only highlights the interplay between a plethora of species, but enables a more rational development of post‐modification of Ti‐containing zeolites.

In the field of electrocatalysis, conductive carbon is commonly incorporated to enhance the electrical conductivity of catalyst materials. However, its specific role in systems involving reconstructed electrocatalysts remains poorly understood, largely due to the complex interplay between carbon surface chemistry and the dynamic reconstruction of catalytic materials. Here, we demonstrate that during the oxygen evolution reaction (OER) under neutral conditions, conductive carbon functions not merely as an electron conductor, but as a critical anchoring platform that facilitates catalyst reconstruction, thereby boosting both the activity and stability of perovskite oxide catalysts. Upon reconstruction, the perovskite oxide releases Co/Fe species, which subsequently redeposit onto the carbon matrix. These redeposited species substantially enhance OER activity and stability through the anchoring effect of carbon. This work provides a new strategy for designing highly stable yet dynamically restructuring OER electrocatalysts by using carbon additives with tailored surface properties.

Transition metal-based electrocatalysts, especially NiFe (oxy)hydroxides, represent state-of-the-art systems for the alkaline oxygen evolution reaction (OER). While structural evolution of electrocatalysts under working conditions has garnered considerable attention, as the evolved structure often dictates catalytic activity, the mechanisms driving these transformations and catalytic performance remain poorly understood. In this work, using NiFe phosphide (NiFeP) as a model system, we systematically elucidate how phosphorus guides irreversible structural transformations and boosts OER performance. Through a combination of electron microscopy, spectroscopy, and electrochemical analysis, we demonstrate that phosphorus facilitates the transformation of NiFeP into NiFe (oxy)hydroxides while retaining residual oxyanion moieties. Importantly, we reveal that phosphorus not only accelerates the active phase formation but also suppresses Fe dissolution and directly modulates the electronic structure, a dual function that has not been well-documented in the literature. The reconstructed catalyst exhibits outstanding OER activity and remarkable stability under alkaline conditions, achieving a low overpotential of 225 mV at 10 mA cm ⁻² and stably maintaining a current density of 500 mA cm ⁻² for over 100 h, ranking among the most effective OER catalysts reported in the literature. Density functional theory calculations indicated that the resulting PO ₄ ³⁻ and Fe act synergistically to regulate the redox chemistry of Ni, preventing Ni over-oxidation and enhancing electronic conductivity. Furthermore, PO ₄ ³⁻ stabilizes key OER intermediates and lower the thermodynamic energy barrier, thereby improving catalytic performance.

The electrocatalytic CO₂ reduction reaction (e-CO₂RR) on Cu-based catalysts has been extensively studied; however, achieving high selectivity for C₂₊ products and long-term durability remains challenging. Here, we introduce a straightforward approach that enhances both C₂H₄ selectivity and catalyst durability by incorporating a nitrogen-rich Schiff-base Network (SNW), leveraging a synergistic interaction between Cu and SNW. Notably, Cu cubes with SNW, predominantly exposing the Cu(200) facet, achieve a Faradaic Efficiency (FE) of 71.2% for C₂H₄ at a current density of 265 mA cm⁻², which not only exceeds tetrahedral and spherical Cu with or without SNW, but also ranks competitively among state‑of‑the‑art Cu-based catalysts reported to date. Theoretical calculations suggest that the presence of SNW on Cu facilitates the *CO-*CHO coupling and/or the C₂H₄ desorption, thereby enhancing C₂H₄ formation. Furthermore, the Cu(200)-SNW surface exhibits optimized Gibbs free energies for the reaction steps compared to bare Cu and other SNW-modified Cu surfaces, which rationalizes the experimental observations. In situ electron microscopy further suggests that SNW confers durability by stabilizing Cu facets and preventing corrosion and dissolution under reaction conditions.