材料科学最新文献

Precise Surface Engineering of Metal Nanoclusters

Ligand programming enables atom-by-atom mastery of metal nanocluster surfaces. Through tailored coordination, interactive ligands, and dynamic interfaces, it shapes adaptive architectures with superior catalytic, optical, and biomedical functions and transforms nanoclusters into intelligent platforms for next-generation materials. More details can be found in the Perspective by Tiankai Chen, Jianping Xie, and co-workers (DOI: 10.1002/adma.202508578).

Designing catalysts that can simultaneously accelerate reactant activation and hydrogenation remains a central challenge in electrochemical ammonia synthesis. Here, a computation-guided, dual-site electrocatalyst design strategy that bridges first-principles theory with device-level validation is reported. Guided by density functional theory, Cu-doped ZnO is identified as an optimal dual-site platform: Cu sites upshift the Zn d-band center, strengthening ^*NO₂ adsorption and enabling facile deoxygenation, while ZnO sites promote water dissociation to supply protons at the reaction interface. This cooperative synergy precisely tunes nitrite activation and hydrogenation kinetics, suppressing competing hydrogen evolution. The resulting catalyst achieves a record NH₃ yield of 552.16 mg h^-1 cm^-2 with 87.9% Faradaic efficiency in a membrane electrode assembly-4× and 18× higher than flow- and H-cell configurations, respectively. Operando spectroscopy confirms the predicted mechanism, demonstrating a theory-to-device workflow that replaces trial-and-error with predictive catalyst design. This approach establishes a generalizable paradigm for developing advanced electrocatalysts for sustainable chemical transformations.

Understanding the microenvironment structure-activity relationship of photo-responsive polymers is crucial to steer the charge carrier flow for molecular oxygen (O₂) activation. However, the spin-forbidden nature of O₂ and the inherent Frenkel exciton effect hinder the efficient O₂ activation, particularly in achieving selective reactive oxygen species (ROSs) generation. Herein, the Sabatier volcano plot is first utilized to manipulate the microenvironment of poly(1,3,5-triethynylbenzene) (PTEB) via molecular defect-mediated charge accumulation to regulate the exciton behavior. The screened PTEB-CN and PTEB-NH₂, with thermodynamic advantages, are created artificial internal electric field (IEF) to induce exciton dissociation and oriented migration. Meanwhile, the significant weakening of exciton binding energy (E_b) in defective PTEBs overcomes the Frenkel exciton effect, switching the O₂ activation from a traditional energy transfer-mediated nonradical route (pristine PTEB) to a hot charge-driven radical pathway. Mechanism inquiry reveals the reversely oriented IEF dictates the migration direction of charge carriers, leading to predominant migration of photo-induced electron (e^-) in conjugated sites toward the ─NH₂ defect, while ─CN defect is primary occupied with photo-induced hole (h⁺). The polarized distribution of charge carriers in PTEB-NH₂ endows the polymeric semiconductor with enhanced selectivity for superoxide radical (O₂ ^•-) generation and improved contaminant removal efficiency. This work offers promising prospective for regulating exciton behavior for organic polymers and opens a frontier for O₂ activation.

Intermetallic nanocatalysts are pivotal for advancing energy conversion and storage technologies. However, their industrial-scale synthesis is fundamentally hindered by the difficulty of maintaining precise compositional and structural control. Here, we introduce a universal phase-engineering strategy, actualized through a continuous roll-flow radiative heating platform that enables the one-step, scalable, and controllable synthesis of highly ordered intermetallic nanocatalysts. This innovative technique demonstrates remarkable versatility, rendering precise fabrication of intermetallic nanocrystals across a vast compositional landscape. Crucially, by modulating key kinetic parameters during synthesis, we achieve precise control over ordering arrangement with fine-tuning of catalytic performance. As a proof of concept, we demonstrate the scalable and sustainable synthesis of nickel-iron intermetallic (Ni₃Fe) nanocatalysts with a predominant L1₂-ordered crystal structure for efficient alkaline water splitting. The resulting catalyst exhibits exceptional electrocatalytic activity, reaching a current density of 10 mA cm^-2 at a low overpotential of 200.2 mV, a performance that rivals the commercial iridium dioxide (IrO₂) benchmark (199.2 mV). Moreover, it shows outstanding long-term durability, with 99.9% current retention over 140 hours and negligible metal leaching. A comprehensive techno-economic evaluation reveals that the hydrogen production cost is strongly dependent on current density, projecting a highly competitive H₂ price as low as $2.33 kg^-1 at 1.0 A cm^-2. This work is expected to provide advanced technology for scalable, sustainable, and continuous manufacturing of intermetallic nanocrystals for economical water splitting.