Rongxing He

Pre‐catalyst reconstruction fundamentally governs the local structure and solid–liquid interface of the derived phase, significantly influencing water electrolysis performance. However, fully unlocking the intrinsic potential of pre‐catalysts remain a persistent bottleneck, as conventional electrolytes cannot functionalize the interface during reconstruction. Herein, we propose an interfacial carbonate‐dominated activation strategy to simultaneously tune the derived NiOOH structure and its interface, enabling efficient oxygen evolution reaction (OER). Using Ca‐Ni ₃ S ₂ as the model pre‐catalyst and K ₂ CO ₃ to replace KOH as the reconstruction electrolyte, the carbonate‐dominated interface kinetically and thermodynamically impedes the transformation of Ni ₃ S ₂ into NiOOH, enabling surface‐confined reconstruction at elevated potential that preserves the interior Ni ₃ S ₂ while forming the functionalized NiOOH phase on the surface. This functionalized surface, induced by the retained CO ₃ ²⁻ from reconstruction, optimizes the electron distribution, interface water framework, and establishes a stable buffer layer, facilitating water oxidation and suppressing NiOOH deactivation. Resultantly, the reconstructed catalyst (Ca‐Ni ₃ S ₂ ‐RC) shows an overpotential of only 261 mV at 100 mA cm ⁻² , a remarkable reduction of 198 mV compared to its KOH‐reconstructed counterpart. Integrated into an alkaline water electrolyzer (AWE), Ca‐Ni ₃ S ₂ ‐RC presents a competitive energy consumption of 4.21 kWh m ⁻³ H ₂ to deliver 4000 A m ⁻² over 900 h, highlighting its promise for industrial applicability.

Pre‐catalyst reconstruction fundamentally governs the local structure and solid–liquid interface of the derived phase, significantly influencing water electrolysis performance. However, fully unlocking the intrinsic potential of pre‐catalysts remain a persistent bottleneck, as conventional electrolytes cannot functionalize the interface during reconstruction. Herein, we propose an interfacial carbonate‐dominated activation strategy to simultaneously tune the derived NiOOH structure and its interface, enabling efficient oxygen evolution reaction (OER). Using Ca‐Ni ₃ S ₂ as the model pre‐catalyst and K ₂ CO ₃ to replace KOH as the reconstruction electrolyte, the carbonate‐dominated interface kinetically and thermodynamically impedes the transformation of Ni ₃ S ₂ into NiOOH, enabling surface‐confined reconstruction at elevated potential that preserves the interior Ni ₃ S ₂ while forming the functionalized NiOOH phase on the surface. This functionalized surface, induced by the retained CO ₃ ²⁻ from reconstruction, optimizes the electron distribution, interface water framework, and establishes a stable buffer layer, facilitating water oxidation and suppressing NiOOH deactivation. Resultantly, the reconstructed catalyst (Ca‐Ni ₃ S ₂ ‐RC) shows an overpotential of only 261 mV at 100 mA cm ⁻² , a remarkable reduction of 198 mV compared to its KOH‐reconstructed counterpart. Integrated into an alkaline water electrolyzer (AWE), Ca‐Ni ₃ S ₂ ‐RC presents a competitive energy consumption of 4.21 kWh m ⁻³ H ₂ to deliver 4000 A m ⁻² over 900 h, highlighting its promise for industrial applicability.

The evolution of optical encryption demands materials that not only conceal information but also enable sophisticated control over its lifecycle. However, increased functionality requires more complex material compositions or device architectures. To circumvent this trade-off, here we report a conceptual and practical evolution from a dual-material binary architecture relying on external erasure to a single-material ternary system featuring intrinsic self-erasure. In the binary design, pristine (C6H8N3)CdCl3 serves as a nonemissive background, while the two addressable states are provided by its N,N-dimethylformamide (DMF)-activated derivative (i.e., (C6H8N3)CdCl3–DMF, green afterglow) and its Mn2+-doped counterpart (no afterglow). This configuration enables dynamic “1/0” readout and selective information erasure upon exposure to water mist. More critically, the Mn2+-doped compound alone functions as a self-contained, multiresponsive unit, manifesting three addressable states under 254 nm irradiation: an initial red state, an HCl-switched green state, and a solvent-induced “off” state. Exploiting these three discrete states affords compact ternary encryption. Furthermore, the latter two states inherently constitute a built-in self-erasure mechanism, enabling complete pattern disappearance without any external intervention. This progression─from combinatorial assembly to integrated functionality─offers a blueprint for designing streamlined, high-capacity optical security platforms.

The lattice of organic–inorganic hybrid metal halides (OIMHs) is predominated by ionic interactions, which leads to spontaneous hydrolysis and structural collapse in water. Most prevailing stabilization approaches tend to either compromise photophysical performance to some extent or involve relatively tedious fabrication routes, failing to reconcile intrinsic water resistance stability with outstanding optoelectronic performance. Herein, we present a “divide‐and‐conquer” molecular interface engineering paradigm based on two typical types of Sn ²⁺ ‐ and Cu ⁺ ‐based OIMHs. For Sn ²⁺ ‐based OIMHs, we propose for the first time a counterintuitive “water‐locking” mechanism that exploits lattice water to build a protective hydrogen‐bond network, maintaining structural integrity in water for over one year. For Cu ⁺ ‐based OIMHs, a “covalent armor” strategy switches the bonding mode from ionic to covalent, anchoring a hydrophobic organic molecular layer onto the inorganic framework to prevent water erosion. Benefiting from these water‐resistant designs, we demonstrate multi‐level information encryption and X‐ray imaging applications, enabling non‐encapsulated underwater X‐ray imaging with a record spatial resolution of 15.5 lp/mm, thereby laying a firm foundation for their practical use in underwater and high‐humidity scenarios.

Electrochemical nitrate reduction to ammonia (NRA) offers a sustainable route for NH3 synthesis. While copper-based catalysts show initial promise for NRA, their performance is fundamentally constrained by insufficient active hydrogen (*H) supply, leading to substantial nitrite accumulation and limited ammonia yields. To overcome this challenge, we report a core–shell Fe2O3@Cu2O pre-catalyst that electrochemically reconstructs under operating conditions into an active Fe3O4/Cu heterojunction with unlocked Fe sites. This catalyst achieves a Faradaic efficiency (FE) of 97.06% at –0.69 V vs. RHE, along with near-complete NO3– conversion (99.08%) and high NH3 selectivity (98.62%). Notably, it maintains robust activity for over 100 h and operates efficiently across a wide nitrate concentration range (14–1000 ppm), achieving a remarkable NH3 production rate of 19,861.83 μg h–1 cm–2 at the highest concentration, which underscores its potential for versatile wastewater treatment. Experimental and theoretical studies reveal a tandem catalytic mechanism: Cu sites adsorb and activate NO3–, while adjacent Fe3O4 sites promote water dissociation to supply *H for the hydrogenation of NO2– intermediates to NH3. Strong interfacial electronic interactions further enhance structural stability. This work provides a design strategy for efficient nitrate-to-ammonia conversion and deepens the mechanistic understanding of tandem electrocatalysis.

Antimony ion doping has been demonstrated as an effective strategy for modulating the photophysics of the host of organic‐inorganic metal halides (OIMHs). The as‐formed doping species exhibit distinct excited‐state dynamics and outstanding photoluminescence efficiency. However, the factors governing emission variations across different host lattices remain unclear. Herein, lattice engineering is employed to elucidate the elusive mechanisms of Sb ³⁺ dopant. Three novel OIMHs—AET‐Cd, AET‐In, and AET‐Sn—featuring central metals (Cd ²⁺ , In ³⁺ , and Sn ⁴⁺ ) with similar electron configuration (4d ¹⁰ 5s ⁰ ) have been prepared to unveil the correlation between host structure and photoluminescence performance. After embedding Sb ³⁺ (4d ¹⁰ 5s ² ) into their lattices, these materials exhibit distinct emission peaks at 590 (AET‐Cd), 567 (AET‐In), and 630 nm (AET‐Sn), respectively. Contrary to the typical ion‐radius‐dependent trend, the emission shifts are attributed to differences in structural distortion and crystal field strength, influenced by both central ion radius and lattice symmetry. Benefitting from their remarkable and tunable photoluminescence properties, applications in second‐harmonic generation response, and anti‐counterfeiting are further demonstrated. Additionally, visible‐light‐communication based on Sb ³⁺ ‐doped materials achieves 2.6 MHz f _‐3 dB with a high data rate of 63 Mbps. These findings provide deep insights into structure‐property relationships and highlight the potential of them in versatile advanced optoelectronic applications.

Nonradiative recombination losses at the interface is a critical bottleneck limiting the performance of perovskite solar cells (PSCs). Self-assembled hole-transporting materials (SA-HTMs) can effectively suppress such recombination, playing a vital role in enhancing device performance. We propose a site-isomeric strategy by introducing dibenzofuran groups into the carbazole unit to design a series of SA-HTMs (DF1CA–DF4CA), from which the most promising molecule was screened via theoretical calculations and subsequently synthesized in a targeted manner. In these designed molecules, theoretical simulated results indicate that DF4CA possesses a conjugated backbone with superior planarity, which can enhance its hole transport ability, interfacial adsorption, and packing density on the ITO substrate, thereby effectively suppressing interfacial nonradiative recombination. Ultimately, the DF4CA-based device achieved a power conversion efficiency of 25.68%, surpassing that of the control device (23.72%), validating the effectiveness of this strategy in regulating interfacial nonradiative recombination and enhancing device performance.

Cyclocarbons constitute a fundamental class of carbon allotropes with unique electronic properties. The recently synthesized C₁₃ provides a crucial model system for understanding odd-numbered cyclocarbons as experimental evidence confirms its dimerization into C₂₆. The underlying mechanism remains unknown, while understanding it is crucial for the synthesis and storage of cyclocarbons. Here, we combine density functional theory with ab initio molecular dynamics simulations to systematically investigate C₁₃ dimerization. Our results identify electronic structures of diverse weakly bound configurations and reveal a nearly barrierless pathway for covalent bond formation of monomers. The reaction proceeds through a general growth-decay mechanism via bridgehead-ring intermediates, ultimately leading to C₂₆. Furthermore, we demonstrate that atomic-scale manipulation of these intermediates may enable the controlled synthesis of various cyclocarbons, including C₇, C₉, C₁₁, C₁₅, C₁₇, and C₁₉. This work provides essential mechanistic insights into cyclocarbon reactivity and establishes a viable bottom-up strategy for the construction of carbon-based nanostructures.

Organic-inorganic hybrid metal halides (OIHMHs) have garnered significant attention for their exceptional photophysical properties and structural diversity. Zero-dimensional (0D) metal halides are particularly promising for anticounterfeiting and solid-state lighting (SSL) due to their outstanding optical properties and stability. However, achieving precise control over the synthesis of low-dimensional OIHMHs (LD-OIHMHs) remains challenging. This study reports the controlled synthesis of Cd²⁺-based OIHMHs, achieving structural dimensionality reduction from 1D to 0D through the strategic embedding of hydrated protons. The 0D structure exhibits an enhanced quantum confinement effect, leading to highly efficient luminescence. Furthermore, Sb³⁺ doping was employed to incorporate optically active centers, resulting in broadband yellow photoluminescence with a large Stokes shift originating from triplet self-trapped excitons in Sb-centered octahedra. The different luminescence properties of these Cd²⁺-based materials were successfully applied in anticounterfeiting. Additionally, a high-performance white light-emitting diode (WLED) was fabricated using the 0D 10% Sb³⁺-doped Cd²⁺-based material as a phosphor, achieving a color rendering index of 90.8 and a luminous efficiency of 43 lm/W, confirming its potential for SSL applications. This work demonstrates an effective strategy for the dimensional and optical engineering of LD-OIHMHs.