Jin-Cheng Liu

Confinement architectures stabilise active metal nanoparticles while preserving molecular accessibility, which proves crucial for heterogeneous catalysis. However, existing methods for preparing encapsulated catalysts such as mesoporous oxides, zeolites, and metal-organic frameworks are costly, complex, and often unreliable. Solid‑state reactions offer a promising alternative, yet conventional pathways yield thermodynamically stable phases that limit activity. Here, we propose a facile, template-free strategy that intercepts amorphous intermediates during solid‑state reactions to form encapsulation layers for active metals. We select ammonia decomposition reaction (ADR, 2NH₃ → N₂ + 3H₂) as the target catalytic reaction, which is a pivotal route to CO_x‑free hydrogen and affords the high‑temperature, reducing environment that drives solid‑state transformations. During ADR conditions, commercial BaCO₃ and Al₂O₃ act as solid‑state reactants, forming Al₂O₃–BaO encapsulation layers around Co or Ni nanoparticles. The layers effectively restrict nanoparticle growth. Amorphous Al₂O₃ facilitates NH₃ adsorption, and amorphous BaO accelerates N₂/H₂ release and enables N–H activation. As a result, the encapsulated catalyst delivers an intrinsic rate of 1,358 mmol H₂·g_metal⁻¹·min⁻¹ that surpasses existing non‑noble metal catalysts, alongside excellent durability during 480 h. This approach offers a blueprint for constructing durable confinement architectures in encapsulated metal catalysts.

As integrated circuit technology scales toward the Angstrom era, the limitations of traditional spin-coated wet photoresists—specifically regarding stochastic defects and pattern collapse—have become critical bottlenecks for high-numerical-aperture extreme ultraviolet (high-NA EUV) lithography. Consequently, dry photoresists deposited via molecular layer deposition (MLD) have emerged as a transformative solution, offering atomic-level thickness control and superior uniformity. Here, we report a tin-based hybrid dry photoresist synthesized via MLD using tetrakis(dimethylamino)tin and 2-butene-1,4-diol. A distinctive feature of this material is its tunable polarity, governed by the development modality: wet development in an ammonia solution yields a positive-tone resist, while dry development using fluorine-based inductively coupled plasma (ICP) etching results in a negative-tone profile. Under 50 keV electron beam exposure (wet development) conditions, we achieved an outstanding resolution limit of 7 nm for a single line, whilst under EUV exposure conditions, we achieved a resolution limit of 18 nm for a single line. To decode the underlying physics of this dual-tone behavior, we employed a rigorous multiscale approach combining in-situ characterization (XPS, TEM, EDS, and EUV-irradiated mass spectrometry) with density functional theory (DFT) calculations. These theoretical and experimental insights elucidate the specific bond-breaking and reorganization mechanisms driving the polarity switch. This work not only presents a high-performance candidate for next-generation lithography but also establishes a fundamental framework for the mechanistic design of advanced dry photoresists.

Periodontitis is a chronic inflammatory disease driven by dynamic microenvironmental imbalances, progressing through successive stages of bacterial infection, immune dysregulation, and tissue destruction. This complex microenvironment exhibits high spatiotemporal heterogeneity, rendering conventional therapies insufficient for stage-specific requirements. This work synthesizes nine-coordinated cerium atomic clusters alongside single atoms anchored on a nitrogen-doped carbon substrate (Ce ACSA@NC). Compared to conventional four-coordinated cerium single-atom structure (Ce SA@NC), Ce ACSA@NC possesses enhanced multi-enzyme mimetic activities, enabling spatiotemporally programed catalytic selectivity aligned with distinct pathological phases. Ce ACSA@NC performs multimodal cascade therapy: rapid antibacterial activity, sustained antioxidant activity, immune regulation, inhibition of bone resorption, and promotion of bone regeneration. Integrated with Pluronic F-127, an injectable thermosensitive hydrogel (Ce ACSA@NC/PF127) ensures precision and durability via staged intervention. This system rapidly eliminates bacteria and scavenges reactive oxygen species (ROS), disrupts the ROS-inflammatory feedback loop, reprograms macrophage polarization, suppresses pro-inflammatory cytokines while enhancing anti-inflammatory secretion, and coordinately modulates the NF-κB pathway and Nrf2 pathways. Through its intrinsic osteogenic properties, Ce ACSA@NC shields bone cells from inflammation, concurrently inhibiting resorption and fostering regeneration. Consequently, the Ce ACSA@NC/PF127 nanoplatform synergistically integrates antibacterial, antioxidant, anti-inflammatory, and osteogenic functions, offering a spatiotemporally adaptive strategy for precision periodontitis therapy with significant clinical potential.

Rare earth hexaborides (REB6) have attracted considerable attention owing to their unique structure. However, the ultrarigid boron cage covalent network within this structure poses immense challenges to the controlled synthesis of their nanocrystals, severely hindering the exploration of their electronic properties and promising application directions. Here we successfully synthesize monodisperse LaB6 nanocrystals with tunable sizes down to sub-20 nm, during which the formation of reactive intermediates and a solution chemistry-like reaction pathway facilitate the formation of monodisperse, small-sized nanocrystals. This strategy is subsequently extended to other rare earth elements, resulting in the establishment of a material library containing 13 types of REB6 nanocrystals. Based on the library, REB6 nanocrystals demonstrate localized surface plasmon resonance (LSPR) properties in the near-infrared region, strongly related to 4f/5d electronic configurations of rare earth elements. Furthermore, they prove to be potentially low-energy photocatalysts under near-infrared light. This study fills a critical gap in systematic research on REB6 nanocrystals, highlighting their promise as a novel class of low-energy near-infrared photocatalysts.

A perennial challenge in nanoengineered catalysis lies in the intrinsic trade-off between maximizing surface reactivity and maintaining structural robustness, which likewise plagues highly active γ-Mo2N-based catalytic materials. Here, we utilized a cryogenic engineering strategy to “freeze” the vulnerable γ-Mo2N surface, coupling with atomically dispersed redox-active Ce1Ox as a dynamic promoter on Pt-γ-Mo2N interfaces. Unlike conventional inert shields that often fail to promote catalytic efficiency, the redox-active Ce1Ox upgraded surface reaction kinetics via electronic modification, meanwhile avoiding irreversible deep oxidation of γ-Mo2N induced by scavenging excessive dissociated *O through reversible redox cycles. We show that integrating a porous, low-temperature passivated Mo2N surface with redox-active Ce1Ox sites dynamically protects against oxidation via reversible Ce3+/Ce4+ cycling while electronically modulating adjacent Pt to enhance CO adsorption and H2O dissociation, thereby achieving both superior activity and exceptional durability in low-temperature hydrogen production. Consequently, the optimized 1Pt-Ce1Ox/Mo2N-194 K catalyst achieves a record-high hydrogen production turnover number of 22,500,000 molH2/molPt alongside outstanding stability exceeding 1500 h in methanol steam reforming. This synergistic approach, merging cryogenic treatment with redox-active shielding, provides a promising paradigm to simultaneously achieve potent catalytic activation and robust structural protection in highly reactive yet inherently vulnerable nanostructures.

Tin-oxo clusters, owing to their exceptionally high extreme ultraviolet (EUV) absorption cross sections, have emerged as promising photoresist materials for EUV lithography, yet their atomic-scale photochemical mechanisms remain poorly understood. Here, by combining density functional theory (DFT) and large-scale molecular dynamics enabled by machine-learning interatomic potentials (MLIPs), we reveal a previously underexplored atomistic pathway for cross-linking in tin-oxo clusters. Beyond conventional Sn–C bond cleavage, cross-linking is strongly influenced by ligand-controlled destabilization of the Sn–O cage framework. Cleavage of Sn–O bonds disrupts cage structural integrity and generates coordinatively unsaturated tin centers that actively facilitate intercluster linkage formation. Notably, the free-energy cost associated with Sn–O bond cleavage is comparable to that of Sn–C dissociation under the same simulation protocol, which identifies framework instability as a driving factor in the structural evolution and cross-linking of tin-oxo photoresists. We further demonstrate that ligand identity critically governs cross-linking behavior by modulating both Sn–C stability and cage resilience: vinyl-functionalized clusters form extensive cross-linked networks containing aggregates up to Sn160 during MLIP molecular dynamics simulation, whereas phenyl ligands largely suppress cross-linking due to stronger Sn–C bonding and steric stabilization. These findings expand the mechanistic picture of tin-oxo photoresist cross-linking and provide atomistic insight for the molecular design of tin-oxo photoresist materials.

Large-language-model agents can now operate the software of computational chemistry, but how their science compares with the answers human experts produced remains untested. Here we present AI Computational Chemist (AICC), a modular skill framework that equips general-purpose agents for computational research: tool-agnostic scientific knowledge, per-code operational skills and orchestration procedures over a machine-readable control plane. We compared an autonomous GPT-5.5 agent, a reference-informed follow-up and the authors’ published computational-content extracts on real referees’ requests from Nature Communications papers, under a fixed document-level rubric executed by two LLM evaluators. The autonomous agent received mean scores of 64.8 and 65.5 of 100, against 72.6 and 54.7 for the published extracts; after one round of human follow-up steering, the same agent scored 69.8 and 72.2. The relative ranking is evaluator-dependent and strongly influenced by differences in documentation completeness. Agent reports scored consistently well on execution reporting and transparency; their principal weaknesses were interpreting reviewer intent and selecting an adequate computational scale.

CeO₂ serves as an essential support or promoter for catalysts in ammonia decomposition, especially those based on Ni, yet its direct contribution to promoting NH₃ activation and H₂ desorption has rarely been understood. Here, we prepare a Ni-Ce-Al trinary catalyst with high-loading (66.5 wt%) Ni nanoparticles. Connected by the Al₂O₃ framework, these Ni nanoparticles are surrounded by abundant atomically dispersed Ce species consisting of Ce single atoms and clusters. The activity-stability trade-off induced by intrinsic Ni sintering on the CeO₂ support is overcome, achieving a high H₂ production rate of 324.0 mmol g_cat^-1 min^-1 at 600 °C. The promoting effect of CeO₂ has been elucidated, originating from the alleviation of hydrogen poisoning. Atomically dispersed Ce species with high hydrogen affinity serve as scavengers for adsorbed H atoms (H^*). The strong tendency to form Ce³⁺‒OH groups facilitates the migration of H^* from Ni nanoparticles to the oxide, releasing poisoned Ni sites and promoting NH₃ activation.