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A major impediment to the development of the efficient use of artificial photosynthesis is the lack of highly selective and efficient photocatalysts toward the conversion of CO2 by sunlight energy at room temperature and ambient pressure. After many years of hard work, we finally completed the synthesis of graphdiyne-based palladium quantum dot catalysts containing high-density metal atom steps for selective artificial photosynthesis. The well-designed interface structure of the catalyst is composed of electron-donor and acceptor groups, resulting in the obvious incomplete charge-transfer phenomenon between graphdiyne and plasmonic metal nanostructures on the interface. These intrinsic characteristics are the origin of the high performance of the catalyst. Studies on its mechanism reveal that the synergism between \'hot electron\' from local surface plasmon resonance and rapid photogenerated carrier separation at the ohmic contact interface accelerates the multi-electron reaction kinetics. The catalyst can selectively synthesize CH4 directly from CO2 and H2O with selectivity of near 100% at room temperature and pressure, and exhibits transformative performance, with an average CH4 yield of 26.2 μmol g-1 h-1 and remarkable long-term stability.

The catalytic activity of platinum for CO oxidation depends on the interaction of electron donation and back-donation at the platinum center. Here we demonstrate that the platinum bromine nanoparticles with electron-rich properties on bromine bonded with sp-C in graphdiyne (PtBr NPs/Br-GDY), which is formed by bromine ligand and constitutes an electrocatalyst with a high CO-resistant for methanol oxidation reaction (MOR). The catalyst showed peak mass activity for MOR as high as 10.4 A mgPt -1, which is 20.8 times higher than the 20 % Pt/C. The catalyst also showed robust long-term stability with slight current density decay after 100 hours at 35 mA cm-2. Structural characterization, experimental, and theoretical studies show that the electron donation from bromine makes the surface of platinum catalysts highly electron-rich, and can strengthen the adsorption of CO as well as enhance π back-donation of Pt to weaken the C-O bond to facilitate CO electrooxidation and enhance catalytic performance during MOR. The results highlight the importance of electron-rich structure among active sites in Pt-halogen catalysts and provide detailed insights into the new mechanism of CO electrooxidation to overcome CO poisoning at the Pt center on an orbital level.

The electrocatalytic reduction reaction of nitrate (NO3 -) to ammonia (NH3) is a feasible way to achieve artificial nitrogen cycle. However, the low yield rate and poor selectivity toward NH3 product is a technical challenge. Here a graphdiyne (GDY)-based tandem catalyst featuring Cu/CuxO nanoparticles anchored to GDY support (termed Cu/CuxO/GDY) for efficient electrocatalytic NO3 - reduction is presented. A high NH3 yield rate of 25.4 mg h-1 mgcat. -1 (25.4 mg h-1 cm-2) with a Faradaic efficiency of 99.8% at an applied potential of -0.8 V versus RHE using the designed catalyst is achieved. These performance metrics outperform most reported NO3 - to NH3 catalysts in the alkaline media. Electrochemical measurements and density functional theory reveal that the NO3 - preferentially attacks Cu/CuxO, and the GDY can effectively catalyze the reduction of NO2 - to NH3. This work highlights the efficacy of GDY as a new class of tandem catalysts for the artificial nitrogen cycle and provides powerful guidelines for the design of tandem electrocatalysts.

Precisely crafting heterojunctions for efficient charge separation is a major obstacle in the realm of photocatalytic hydrogen evolution. A 0D/2D heterojunction was successfully fabricated by anchoring Ag2S quantum dots (Ag2S QDs) onto graphdiyne (GDY) nanosheets (Ag2S QDs/GDY) using a straightforward physical mixing technique. This unique structure allows for excellent contact between GDY and Ag2S QDs, thereby enhancing the rate of charge transfer. The light absorption capabilities of Ag2S QDs/GDY extend up to 1200 nm, enabling strong absorption of light, including infrared. Through DFT calculations and in-situ XPS analysis, it was demonstrated that incorporating Ag2S QDs onto GDY effectively modulates the electronic structure, promotes an internal electric field, and facilitates directional electron transfer. This directed electron transfer enhances the utilization of electrons by GDY and Ag2S QDs, with the added benefit of Ag2S QDs serving as electron reservoirs for efficient photocatalytic hydrogen evolution. A 7 %Ag2S QDs/GDY composite exhibited impressive efficiency and stable performance in photocatalytic hydrogen evolution (2418 μmol g-1 h-1), which is much higher than that of GDY and Ag2S QDs. This study conclusively demonstrates that the 0D/2D heterojunction formed by GDY and Ag2S QDs can establish high-quality contact and efficient charge transfer, ultimately enhancing photocatalytic performance.

Metal atom catalysts have been among the most important research objects due to their specific physical and chemical properties. However, precise control of the anchoring of metal atoms is still challenging to achieve. Cobalt and iridium atomic arrays formed sequentially ordered stable arrays in graphdiyne (GDY) triangular cavities depending on their intrinsic chemical properties and interactions. The success of this method was attributed to multifunctional integration of GDY, enabling selective growth from one to several atoms and various atomic densities. The bimetallic atom arrays show several advantages resulting from reducibility of acetylene bonds, space limiting effect, incomplete charge transfer between GDY and metal atoms, and sp-C hybridized triple bond skeleton. This well-designed system exhibits unprecedented oxygen evolution reaction (OER) performance with a mass activity of 2.6 A mgcat. -1 at a low overpotential of 300 mV, which is 216.6 times higher than the state-of-the-art IrO2 catalyst, and long-term stability.

The performance of zinc-air battery is constrained by the sluggish rate of oxygen electrode reaction, particularly under high current discharge conditions where the kinetic process of the oxygen reduction reaction (ORR) decelerates significantly. To address this challenge, we present a novel phase transition strategy that facilitates the creation of a heteroatom-doped heterointerface (CoN/CoS2). The meticulously engineered CoN/CoS2/NC electrocatalyst displays a superior ORR half-wave potential of 0.87 V and an OER overpotential of 320 mV at 10 mA cm-2. Experimental and computational analysis confirm that the CoN/CoS2 heterostructure optimizes local charge distribution, accelerates electron transfer, and tunes active sites for enhanced catalysis. Notably, this heterojunction improves stability by resisting corrosion and degradation under harsh alkaline conditions, thus demonstrating superior performance and longevity in a custom-made liquid zinc-air battery. This research provides valuable practical and theoretical foundations for designing efficient heterointerfaces in electrocatalysis applications.

Photothermal modulation of neural activity offers a promising approach for understanding brain circuits and developing therapies for neurological disorders. However, the low neuron selectivity and inefficient light-to-heat conversion of existing photothermal nanomaterials significantly limit their potential for neuromodulation. Here, we report that graphdiyne (GDY) can be developed into an efficient neuron-targeted photothermal transducer for in vivo modulation of neuronal activity through rational surface functionalization. We functionalize GDY with polyethylene glycol (PEG) through noncovalent hydrophobic interactions, followed by antibody conjugation to specifically target the temperature-sensitive transient receptor potential cation channel subfamily V member 1 (TRPV1) on the surface of neural cells. The nanotransducer not only exhibits high photothermal conversion efficiency in the near-infrared region but also shows great TRPV1-targeting capability. This enables photothermal activation of TRPV1, leading to neurotransmitter release in cells and modulation of neural firing in living mice. With its precision and selectivity, the GDY-based transducer provides an innovative avenue for understanding brain function and developing therapeutic strategies for neurodegenerative diseases.

The accurate construction of composite material systems containing graphdiyne (GDY) and other metallic materials has promoted the formation of innovative structures and practical applications in the fields of energy, catalysis, optoelectronics, and biomedicine. To fulfill the practical requirements, the precise formation of multiscale interfaces over a wide range, from single atoms to nanostructures, plays an important role in the optimization of the structural design and properties. The intrinsic correlations between the structure, synthesis process, characteristic properties, and device performance are systematically investigated. This review outlines the current research achievements regarding the controlled formation of multiscale metallic interfaces on GDY. Synthetic strategies for interface regulation, as well as the correlation between the structure and performance, are presented. Furthermore, innovative research ideas for the design and synthesis of functional metal-based materials loaded onto GDY-based substances are also provided, demonstrating the promising application potential of GDY-based materials.

Cu2+ accelerates the viral-like propagation of α-synuclein fibrils and plays a key role in the pathogenesis of Parkinson\'s disease (PD). Therefore, the accurate detection of Cu2+ is essential for the diagnosis of PD and other neurological diseases. The Cu2+ detection process is impeded by substances that have similar electrochemical properties. In this study, graphdiyne (GDY), a new kind of carbon allotrope with strong electron-donating ability, was utilized for the highly selective detection of Cu2+ by taking advantage of its outstanding adsorption capacity for Cu2+. Density functional theory (DFT) calculations show that Cu atoms are adsorbed in the cavity of GDY, and the absorption energy between Cu and C atoms is higher than that of graphene (GR), indicating that the cavity of GDY is favorable for the adsorption of Cu atoms and electrochemical sensing. The GDY-based electrochemical sensor can effectively avoid the interference of amino acids, metal ions and neurotransmitters and has a high sensitivity of 9.77 μA·μM-1·cm-2, with a minimum detectable concentration of 200 nM. During the investigating pathogenesis and therapeutic process of PD with α-synuclein as the diagnostic standard, the concentration of Cu2+ in cells before and after L-DOPA and GSH treatments were examined, and it was found that Cu2+ exhibits high potential as a biomarker for PD. This study not only harnesses the favorable adsorption of the GDY and Cu2+ to improve the specificity of ion detection but also provide clues for deeper understanding of the role of Cu2+ in neurobiology and neurological diseases.