The molecular mechanism of interfacial polymerization remains elusive due to rapid kinetics and nanoscale heterogeneity, while existing simulations struggle to balance chemical reactivity with computational efficiency. To address this, we developed the "Interfacial Polymerization Simulator" (IPS), an automated framework coupled with LAMMPS that models the continuous reaction-diffusion process via dynamic topology updating and explicit solvent handling. Specifically, IPS employs a novel dynamic region partitioning scheme for real-time regulating monomer concentrations. Applying this method to the m-phenylenediamine and trimesoyl chloride system, we reveal a "trunk-growth" mechanism where initial heterogeneous protrusions evolve into a dense layer with intrinsic voids. Furthermore, thermal curing simulations quantitatively reproduced structural densification (reaching ∼84% cross-linking degrees), yielding density and pore size distributions consistent with experimental benchmarks. IPS provides a robust, efficient computational tool for elucidating reaction mechanisms and guiding the rational design of functional materials synthesized by interfacial polymerization.

The transition toward sustainable chemical production necessitates highly efficient catalysts for both fossil fuel and biomass conversion. Zeolites, with their crystalline frameworks, tunable pore structures, and well-defined acid sites, offer unparalleled opportunities for selective catalysis in processes ranging from methanol-to-olefins (MTO) and methanol-to-aromatics (MTA) to fluid catalytic cracking (FCC) and biomass upgrading. Solid-state nuclear magnetic resonance (NMR) uniquely enables atomic-level insights into framework connectivity, acid site distribution, and host-guest interactions. This review systematically summarizes the application of various NMR methodologies for zeolite characterization, including probing Brønsted and Lewis acidity, framework topology, and porosity across diverse zeolite topologies. By highlighting these NMR-based strategies, the review provides a comprehensive guide for understanding structure-function relationships in zeolite catalysts and their rational design for sustainable chemical processes.

This review summarizes alkaline water electrolysis for industrial green hydrogen, highlighting catalyst design, AI/DFT optimization, and full-cell engineering to overcome mass-transport and durability limits toward high-current operation.

Deactivation of supported metal nanoparticles due to sintering is a key issue in industrial catalysts. We report an efficient, low-cost protocol for producing highly active and robust heterogeneous catalysts with low palladium loading (1.3%), high dispersion, and resistance to sintering. This is achieved using ethylenediamine (EN) as an inexpensive bidentate ligand for in situ complexation of Pd(II) ions in water, promoting stable impregnation and higher dispersion on a fumed silica support. Following EN decomposition in air at 225 degrees C for 48 h and subsequent hydrogen reduction, CO and H2 chemisorption revealed a marked increase in Pd dispersion, from 6% at molar ratio n = 0 to 30% at n = 4, plateauing at n = 4-6, for this set of Pd:nEN samples. These Pd nanoparticles showed excellent catalytic activity and stability for propylene hydrogenation at 250 degrees C. Consistent with the trend in dispersion, catalytic activity increased with increasing Pd:nEN ratio from n = 0 to 4, then plateaued at 93% for n = 4-6. Testing under higher space velocity confirmed that the catalyst retained both high activity and stability. In summary, EN could be an industrially applicable ligand that yields a fumed silica-supported Pd catalyst suitable for hydrogenation.

Carbon dots (CDs), as a novel class of fluorescent nanomaterials, have demonstrated significant potential in tumor theranostics due to their outstanding optical properties, excellent biocompatibility, and ease of surface functionalization. However, the clinical translation and functional optimization of CDs remain significantly limited due to the strong dependence of their structural and physicochemical properties on synthetic parameters, particularly the nature of carbon precursors and the strategies adopted for elemental doping. Herein, this review systematically summarizes recent progress in the design and synthesis of CDs derived from diverse precursors, including bulk carbon materials, small organic molecules (such as organic acids, near-infrared dyes, aromatic compounds, and amines), and biomass-based sources (plant-derived substances and animal by-products). Particular attention is given to the influence of precursor molecular structure on particle size, surface chemistry, fluorescence behavior, and biological interactions. Through the integration of diverse synthetic methodologies and structural engineering strategies, this review examines the current requirements for functional refinement and delineates the principal limitations associated with the application of CDs in tumor diagnosis and therapy. Therefore, this review provides a solid theoretical and practical basis for the development of efficient, safe, and clinically applicable carbon dot nanoplatforms, and establishes a foundation for precise and personalized cancer diagnosis and treatment.

The nonoxidative coupling of methane (NOCM) offers a promising route to convert methane into value-added chemicals. Liquid metals have emerged as potential catalysts for NOCM, due to their propensity against coke formation and the flexible atomic arrangement that facilitates methane activation, with liquid state indium (In) gaining attention. However, the reaction pathways and catalytic mechanisms of In during NOCM have yet to be fully understood. Here, we report the discovery of locally generated In liquid metal active sites on In2O3 for the NOCM reaction, supported by silicon dioxide substrates, in the vicinity of an in situ formed In silicon oxide (In2Si2O7) interfacial layer. By the implementation of combined in situ transmission electron microscopy and electron energy loss spectroscopy, we directly observed the formation of liquid metal "In active sites", near the interfacial layer, at >600 °C. The spectroscopy analysis reveals that In2Si2O7 is a reservoir in methane conversion, storing reactive H* and CH x * intermediate spillover from "In" for driving the NOCM reaction, avoiding the overcracking of CH4 over metallic In. This finding provides a practical approach for the rational design of efficient and noncorrosive liquid metal-based catalysts.

Flame-spray pyrolysis forms surface-distorted Al V species that interact with silanols to create strong Brønsted acid sites, markedly enhancing the acidity and catalytic performance of amorphous silica–alumina.

The conversion of methane over zeolite catalysts is governed by the interplay of framework topology and aluminum siting, yet a predictive design framework is lacking. Here, we demonstrate that the synergy between pore architecture and specific aluminum siting, revealed by 27 Al MQMAS/MAS NMR, steers methane valorization as a "molecular traffic controller". In zeolites with 1D, 2D, and 3D topologies, this synergy dictates product distribution: methanol dominates at low temperatures with the activity order FER > TON > MFI, while at moderate temperatures, 1D channels maintain methanol, 2D channels co-produce dimethyl ether, and 3D channels enable tandem conversion to olefins and aromatics. We derive guiding principles: match aluminum siting to transition-state confinement; tune channel dimensionality to control reaction depth; and avoid exposing Al sites in 10-ring channels at high temperatures to prevent over-oxidation. This work establishes a design blueprint for methane conversion catalysts in sustainable C1 chemistry.

ABSTRACT The carbon dioxide dry reforming of methane (DRM) is a promising technology for achieving carbon neutrality via the simultaneous conversion of two greenhouse gases (CH 4 and CO 2 ) into high‐value syngas. However, its industrial implementation is severely hindered by its highly endothermic nature and the rapid catalyst deactivation originating from metal sintering and carbon deposition. This review provides a comprehensive analysis of DRM technology, linking fundamental surface steps to advanced catalyst design strategies. It begins by clarifying the inherent thermodynamic and kinetic constraints, detailing the reactant activation, and uncovering the essence of catalyst deactivation. The design strategies for synthesizing durable and cost‐effective DRM catalysts are categorized into two dimensions: active site engineering (e.g., particle downsizing, bimetallic alloying, and promoter incorporation) and functional support modulation (e.g., acidity–basicity adjustment, oxygen vacancy generation, and multi‐functional confinement). Finally, this review proposes a multi‐dimensional roadmap for future commercialization. We emphasize the integration of data‐driven machine learning (ML), energy‐assisted catalysis, macroscopic process intensification, and techno‐economic analyses. This holistic perspective aims to bridge the gap between laboratory‐scale concepts and industrial feasibility, positioning DRM as a cornerstone technology of the sustainable chemical industry.

Cu/ZnO/ZrO2 (CZZ) catalysts are widely used in CO2 hydrogenation to methanol. However, their structural dynamics under reaction conditions and related reaction mechanism remain unclear. In this study, we employed in-situ transmission electron microscopy (TEM) to investigate structural changes in Cu/ZnO/ZrO2 catalysts under CO2 and H2/CO2 environments at 200 degrees C and 250 degrees C. Under CO2 conditions, coexisting CuO and ZnO phases were observed along with a diminishing crystalline ZrO2 phase. Under H2/CO2 conditions, dynamic formation and evolution of a CuZn alloy phase occurred, accompanied by the reappearance of crystalline ZrO2 nano-particles. It is also noted that copper in Cu/ZnO/ZrO2 is difficult to be completely reduced in a H2/CO2 environment, in contrast to un-supported CuO nanoparticles. These results suggest a distinct function of ZrO2 and ZnO support in the catalyst, which alters the catalytic performance of the CZZ system. The findings of this study provide new insight into the dynamic behavior of CZZ catalysts under actual reaction conditions.

As an important chemical raw material, ammonia is of great significance in fertilizer production and hydrogen energy storage. Ammonia synthesis via the Haber-Bosch process has been under continuous development for over a century, with previous studies predominantly emphasizing the electron donation effect from the support. However, various phenomena hint at other support effects also contributing to this reaction, while the detailed mechanism is yet to be fully discovered. This research reveals an additional role of the supports and an alternative reaction pathway to boost the ammonia synthesis, based on in situ environmental transmission electron microscopy and electron energy loss spectroscopy (EELS) investigation of two selected model catalysts, Ru/MgO and Ru/Al2O3. The activation and dissociation of N2 and H2 molecules occurred on Ru particles to generate active N* and H* species. During the reaction, the in situ-generated oxygen defects on MgO act as an N* reservoir to form the Mg-N* interaction, as evidenced by both in situ EELS and diffuse reflectance infrared Fourier-transform spectroscopy. The density functional theory calculation confirmed that the dissociated N* over the Ru particle will automatically refill into the surface oxygen defects on MgO due to the lower refilling energy. Thus, the support not only extracts the active N* from the Ru surface by nitrogen spillover, thereby suppressing N* recombination to N2, but also promptly frees Ru active sites for subsequent activation. This strongly enhances the reaction rate of N2 activation and dissociation, and further boosts the ammonia productivity.

Nano enzyme catalysts are an emerging class of heterogeneous catalysts that translate enzymatic concepts such as site isolation, cooperative motifs, second-sphere interactions and microenvironment regulation into robust solids for the selective transformation of carbon-centred molecules under practical conditions. This review defines nano enzyme catalysts and distinguishes them from biomedical nanozymes, then summarises design principles that link atomic-scale active site construction and microenvironment engineering to reaction pathway control in carbon conversion. Mechanistic descriptors from enzymology and surface catalysis are compared to clarify when Michaelis-Menten type saturation behaviour reflects an enzyme-like catalytic cycle and when it more likely originates from adsorption or surface coverage limitations. Key strategies are discussed in the context of stabilising critical intermediates while suppressing deep oxidation, overhydrogenation and coke formation. These strategies include single-atom sites and sub-nanoclusters, defect and vacancy anchoring, confinement within porous frameworks and regulation of local hydrophilicity or hydrophobicity together with proton and electron transfer. Synthesis routes and representative thermal catalytic case studies are reviewed, followed by remaining challenges in operando active site identification, quantitative microenvironment descriptors, scalable synthesis and long-term stability.

Plastic waste is abundant in carbon and hydrogen resources. The development of sustainable catalytic process for the recovery of chemicals from waste plastic offers a promising strategy to simultaneously mitigate environmental pollution and reduce dependence on petrochemical products. Among the valuable targets, aromatic chemicals are particularly attractive which are widely used in polymers, pharmaceuticals, and fuels. Therefore, photocatalytic recovery of aromatic chemicals from waste plastic attracts huge attention to contribute to sustainable technology and circular economy, which couple solar energy with catalyst-controlled redox chemistry to enable plastic upcycling under mild conditions. In this Review, the fundamentals of photocatalytic plastic upcycling are outlined, including photocatalytic mechanism and the thermodynamic and kinetic challenges. Then, representative catalytic systems are discussed, such as polyethylene terephthalate, polystyrene, and polyphenylene sulfide. Finally, the future challenges and development directions are summarized, including development of catalytic system, mechanistic elucidation, real-world plastic feedstocks, and techno-economic analysis. This Review provides a comprehensive framework for understanding photocatalytic aromatic chemical recovery from waste plastic and offers guidance for the rational design of efficient, selective, and scalable solar-driven upcycling systems.

Selective catalytic oxidation of ammonia (NH3-SCO) to N-2 is crucial for abating residual NH3 emissions, but existing catalysts struggle to combine low-temperature activity with high N-2 selectivity due to competitive Pt-NO interactions. Here we design a tandem confinement catalyst by depositing sub-nanometer Pt clusters (similar to 0.72 nm) inside the supercages of a Cu-exchanged USY zeolite via atomic layer deposition (ALD), creating intimately paired Pt-Cu active sites. This confined Pt/Cu-USY ALD catalyst achieves >90 % NH3 conversion and >90 % N-2 selectivity across an exceptionally broad 170-300 degrees C window under simulated exhaust conditions, surpassing all previously reported Pt-based NH3-SCO catalysts. The simultaneously enhanced low-temperature activity and high-temperature N-2 selectivity of the Pt/Cu-USY ALD catalyst can be attributed to the spatial confinement of Pt clusters within the Cu-USY framework, which leads to an expanded NO desorption window (150-350 degrees C). Detailed in situ studies further reveal that N2O4 species preferentially serve as NO storage intermediates on the Pt/Cu-USY ALD catalyst surface at low temperatures, exhibiting significantly lower formation barriers compared to free nitrates, which dominate as intermediates in conventional Pt-Cu systems. This effectively mitigates free nitrate-induced site poisoning and overcomes the typical activity-selectivity trade-offs observed in conventional Pt-Cu dual-site catalysts.

Amid escalating CO2 emissions and their dire environmental impacts, this study rigorously assesses the technical feasibility of sustainable industrial methanol production via CO2 hydrogenation by integrating a sensitivity analysis and life cycle assessment (LCA). This work novelly examines the interconnections between economic, environmental, and operational factors to better understand the process improvements. By leveraging process and economic simulations in Aspen Plus and Aspen Process Economic Analyzer, process conditions of 220 degrees C, 98 bar, and 3:1 H2:CO2 feed maximized the process efficiency (98.1 % CO2 conversion, 99.9 % methanol selectivity, and 98.1 % methanol yield) and achieved a competitive production cost of 0.534 USD2023 kgMeOH-1 , undercutting the conventional price (0.552 USD2023 kgMeOH-1 ). Incorporating green instead of grey hydrogen increased the production cost to 0.78 USD2023 kgMeOH-1 and simultaneously reduced the carbon footprint from 2.29 to 0.32 kgCO2 kgMeOH-1 and further to 0.03 kgCO2 kgMeOH-1 if using additional renewable resources. We conclude that while this process is technically feasible and could potentially align with carbon neutrality and circular economy strategies, further research into sustainable hydrogen sources, effective CO2 capture technologies, improved catalyst design, access to renewable energy, ideal policy interventions, and practical applications, such as pilot plants, are essential for effective large-scale commercialization.

CO2 reforming of methane, also known as dry reforming of methane, offers promising prospects for the catalytic conversion of CO2 and CH4 to produce H2, but low-cost catalysts with high activity and stability in operation under severe conditions are needed. We now report such a catalyst, consisting of copper-nickel nanoparticles on a support. The catalyst operated with high activity for more than 1200 h of continuous operation in a flow reactor with a feed of CH4:CO2:N2 in a molar ratio of 1:1:1. In-situ X-ray absorption spectra show that the catalyst consisted of a dilute alloy of copper in nickel during operation, being resistant to metal sintering and the formation of carbonaceous deposits even at 700 °C. The data are consistent with the suggestion that the catalyst was a single-atom alloy and point to the possibility of a range of applications of such catalysts.

The simultaneous utilization of photoelectrons and holes to achieve the coupling of photocatalytic hydrogen evolution with the selective oxidation of organic substances holds significant importance. Yet, this strategy is often constrained by the inadequate charge separation efficiency of photocatalysts and the scarcity of sufficient catalytic active sites. Herein, a conductive bimetallic metal-organic framework (MOF), CuxNi1-x-HHTP, was strategically integrated onto the surface of CdS nanorods, yielding a visible-light-responsive CdS@CuxNi1-x-HHTP core-shell inorganic-organic hybrid, which demonstrated exceptional performance and remarkable product selectivity in the photocatalytic dehydrogenative coupling of benzylamine. The incorporation of CuxNi1-x-HHTP endows the photocatalytic system with a plethora of accessible reactive sites. Moreover, the ultrafast spectroscopy research unveils that Cu0.5Ni0.5-HHTP exhibits robust capability for efficient photogenerated electron extraction, thereby effectively facilitating the spatial separation of photogenerated carriers during the photocatalytic process. Notably, when the CdS/Cu0.5Ni0.5-HHTP molar ratio was 1:2 in photocatalysts, the catalyst denoted as CdS@Cu0.5Ni0.5-HHTP-2 demonstrated a remarkable hydrogen evolution rate of 29.79 mmol g- 1 h- 1, accompanied by a benzylamine conversion rate of 58.39%, while maintaining high stability. This study introduces a strategy for integrating conductive bimetallic metal-organic frameworks with inorganic semiconductors, enabling ultrafast photocarrier transfer and significantly enhancing photocatalytic efficiency.

Lignocellulosic biomass can replace a portion of the petroleum and fossil fuel feedstocks. It is used in the production of biofuels (e.g., bioethanol) and platform chemicals (e.g., HMF, furfural), enabling the sustainable production of fuels and value-added chemicals. Differentiating from traditional thermochemical and biochemical processes, photocatalysis is emerging as a more straightforward and environmentally friendly pathway for biomass conversion. This approach drives biomass transformations using photo-excited charge carriers and photo-generated reactive species, resulting in distinct reaction pathways. Under mild conditions, photocatalysis allows the selective functionalization of targeted functional groups and the precise cleavage of specific chemical bonds. This review provides an overview of photo reactions involving the conversion of glucose or fructose to HMF, and subsequent transformation of HMF into value-added chemicals under visible or UV light irradiation, clarifying the underlying mechanisms. Potential strategies for the photocatalytic conversion of sugars are also discussed, with key challenges that should be addressed to enhance economic viability and long-term sustainability.

The CO2 dry reforming of methane (DRM) to produce hydrogen-rich syngas offers a promising solution transforming two major greenhouse gases into a high-value product. DRM has the potential for commercial application, but the limited stability of catalysts poses a significant barrier to its widespread application. Flame spray pyrolysis (FSP) has emerged as an innovative technique for designing catalysts with distinct structures that enhance both activity and durability. In this study, double-flame spray pyrolysis (DF-FSP) has been utilized to design cobalt-based nanoparticles on an alumina support. The DF-FSP results in the formation of an interfacial layer of CoxAlyO4, which acts as an adhesive layer between the cobalt nanoparticles and the Al2O3 support. This interfacial layer stabilizes the cobalt active sites for over 80 h during DRM at 700 °C, achieving a CO2 conversion rate of 68.6%. In contrast, a conventionally synthesized Co/Al2O3 catalyst, lacking this interfacial layer, exhibited complete deactivation within 7 h and a maximum CO2 conversion of 67.7%. The DF-FSP thus presents a compelling alternative for synthesizing catalysts with interfacial stable adhesive layers, resulting in state-of-the-art performance for challenging catalytic reactions.