The development of high-performance atomic catalysts for the carbon dioxide reduction reaction (CO₂RR) is a time-consuming process due to the complexity of the reaction mechanism and the uncertainty of the active site. Herein, we have proposed combining density functional theory (DFT) and machine learning (ML) to investigate the potential of topological graphene-based dual-atom catalysts (DACs) as CO₂RR electrocatalysts. By analyzing the ML results, we identify the number of d-orbital electrons in the active site as a key factor influencing the CO₂RR catalytic activity. Additionally, we propose a simple descriptor to measure the CO₂RR activity of these DACs. Our findings provide plausible explanations for the synergistic interactions between bimetallic atoms in CO₂RR and allow us to screen the homogeneous Ni-Ni pair as the most promising dual-atom catalysts. This work offers a fast ML approach based on limited DFT calculations to predict the most electroactive and stable DACs on carbon support for CO₂RR, facilitating rapid screening of high-performance dual-atom catalysts.

Currently, dual atomic catalysts (DACs) with neighboring active sites for oxygen reduction reaction (ORR) still meet lots of challenges in the synthesis, especially the construction of atomic pairs of elements from different blocks of the periodic table. Herein, a “rare earth (Ce)-metalloid (Se)” non-bonding heteronuclear diatomic electrocatalyst has been constructed for ORR by rational coordination and carbon support defect engineering. Encouraging, the optimized Ce-Se diatomic catalysts (Ce-Se DAs/NC) displayed a half-wave potential of 0.886 V vs. reversible hydrogen electrode (RHE) and excellent stability, which surpass those of separate Ce or Se single atoms and most single/dual atomic catalysts ever reported. In addition, a primary zinc-air battery constructed using Ce-Se DAs/NC delivers a higher peak power density (209.2 mW·cm⁻²) and specific capacity (786.4 mAh·g_Zn⁻¹) than state-of-the-art noble metal catalysts Pt/C. Theoretical calculations reveal that the Ce-Se DAs/NC has improved the electroactivity of the Ce-N₄ region due to the electron transfer towards the nearby Se specific activity (SA) sites. Meanwhile, the more electron-rich Se sites promote the adsorptions of key intermediates, which results in the optimal performances of ORR on Ce-Se DAs/NC. This work provides new perspectives on electronic structure modulations via non-bonded long-range coordination micro-environment engineering in DACs for efficient electrocatalysis.

Rare-earth (RE) halide solid electrolytes (HSEs) have been an emerging research area due to their good electrochemical and mechanical properties for all-solid-state lithium batteries (ASSBs). However, only very limited types of HSEs have been reported with high performance. In this work, tens of grams of RE-HSE Li₃TbBr₆ (LTbB) was synthesized by a vacuum evaporation-assisted method. The as-prepared LTbB displays a high ionic conductivity of 1.7 mS·cm⁻¹, a wide electrochemical window, and good formability. Accordingly, the assembled solid lithium-tellurium (Li-Te) battery based on the LTbB HSE exhibits excellent cycling stability up to 600 cycles, which is superior to most previous reports. The processes and the chemicals during the discharge/charge of Li-Te batteries have been studied by various in situ and ex situ characterizations. Theoretical calculations have demonstrated the dominant conductivity contributions of the direct [octahedral]–[octahedral] ([Oct]–[Oct]) pathway for Li ion migrations in the electrolyte. The Tb sites guarantee efficient electron transfer while the Li 2s orbitals are not affected during migration, leading to a low activation barrier. Therefore, this successful fabrication and application of LTbB have offered a highly competitive solution for solid electrolytes in ASSBs, indicating the great potential of RE-based HSEs in energy devices.

Currently, single-atom combo catalysts (SACCs) for carbon dioxide reduction reaction (CO₂RR) to the formation of HCOOH are still very limited, especially the lanthanide-based SACCs. In this work, the novel SACCs with atomically dispersed In and Ce active sites were successfully prepared on the nitrogen-doped carbon matrix (InCe/CN). Both aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM) images and the extended X-ray absorption fine structure (EXAFS) spectra proved the well-isolated In and Ce atoms. The as-prepared InCe/CN shows a high Faradaic efficiency (FE) (77%) and current density of HCOOH formation (j_HCOOH) at −1.35 V vs. reversible hydrogen electrode (RHE), much higher than the single atom catalysts. Theoretical calculations have indicated that the introduced Ce single atom sites not only significantly promote electron transfer but also optimize the In-5p orbitals towards higher selectivity towards the HCOOH formation. This work innovatively extends the design of SACCs towards the main group and Ln metals for more applications.

Solid-state Li metal batteries with solid electrolytes have built a potential way to solve the safety and low energy density problems of current commercial Li-ion batteries with liquid electrolyte. As a key component of solid-state Li metal batteries, solid electrolytes require high ionic conductivities and good mechanical properties. We have designed a composite solid electrolyte (CSE) consisting of poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP)-Li_6.5La₃Zr_1.5Ta_0.5O₁₂ (LLZTO)-succinonitrile (SN) and Li bis(trifluoromethylsulphonyl)imide (LiTFSI). The PVDF-HFP-based porous matrix made by electrospinning ensures good mechanical properties of the electrolyte membrane, and the large proportion of SN filling material makes the electrolyte membrane have an ionic conductivity of 1.11 mS·cm^–1 without the addition of liquid electrolyte. The symmetric battery assembled with CSE can be cycled stably for more than 600 h, and the LiFePO₄|CSE|Li full battery can also be cycled stably for more than 200 cycles. In addition to Li metal batteries, Li-O₂ and Li-CO₂ batteries that use CSE as electrolytes also have good performances, reflecting the universality of CSE. CSE does not only guarantee good mechanical properties but also obtain a high ionic conductivity. This design provides a new idea for the commercial application of polymer-based solid batteries.

Iron-based nanostructures represent an emerging class of catalysts with high electroactivity for oxygen reduction reaction (ORR) in energy storage and conversion technologies. However, current practical applications have been limited by insufficient durability in both alkaline and acidic environments. In particular, limited attention has been paid to stabilizing iron-based catalysts by introducing additional metal by the alloying effect. Herein, we report bimetallic Fe₂Mo nanoparticles on N-doped carbon (Fe₂Mo/NC) as an efficient and ultra-stable ORR electrocatalyst for the first time. The Fe₂Mo/NC catalyst shows high selectivity for a four-electron pathway of ORR and remarkable electrocatalytic activity with high kinetics current density and half-wave potential as well as low Tafel slope in both acidic and alkaline medias. It demonstrates excellent long-term durability with no activity loss even after 10,000 potential cycles. Density functional theory (DFT) calculations have confirmed the modulated electronic structure of formed Fe₂Mo, which supports the electron-rich structure for the ORR process. Meanwhile, the mutual protection between Fe and Mo sites guarantees efficient electron transfer and long-term stability, especially under the alkaline environment. This work has supplied an effective strategy to solve the dilemma between high electroactivity and long-term durability for the Fe-based electrocatalysts, which opens a new direction of developing novel electrocatalyst systems for future research.

Mechanoluminescence (ML) has become the most promising material for broad applications in display and sensing devices, in which ZnS is the most commonly studied one due to its stable and highly repetitive ML performances. In this work, we have successfully prepared the biphase ZnS on a large scale through the facile in-air molten salt protection strategy. The obtained biphase has the best ML properties, which is mainly attributed to the synergistic effects of piezo-photonic, defect, and interface dislocations. DFT calculations have confirmed that the defects activate the local S and Zn sites and reduce the energy barrier for electron transfer. The much stronger X-ray induced luminescence than the commercial scintillator is also reached. The application of ZnS particles in both papers and inks delivers superior performance. Meanwhile, ZnS particles based screen printing ink is able to directly print on paper, plastic and other carriers to form clear marks. These proposed paper and ink hold great potentials in applications of information security and anti-counterfeiting based on the multi-mode luminescence properties. This work provides a new avenue to understand and realize the high-performance multi-mode luminescence, inspiring more future works to extend on other ML materials and boosting their practical applications.

The on-surface self-assembly of inorganic atomic clusters and organic molecules offers significant opportunities to design novel hybrid materials with tailored functionalities. By adopting the advantages from both inorganic and organic components, the hybrid self-assembly molecules have shown great potential in future optoelectrical devices. Herein, we report the co-deposition of 4,8-diethynylbenzo[1,2-d-4,5-d0]bisoxazole (DEBBA) and Se atoms to produce a motif-adjustable organic–inorganic hybrid self-assembly system via the non-covalent interactions. By controlling the coverage of Se atoms, various chiral molecular networks containing Se, Se ₆, Se₈, and terminal alkynes evolved on the Ag(111) surface. In particular, with the highest coverage of Se atoms, phase segregation into alternating one-dimensional chains of non-covalently bonded Se₈ clusters and organic ligands has been noticed. The atom-coverage dependent evolution of self-assembly structures reflects the remarkable structural adaptability of Se clusters as building blocks based on the spontaneous resize to reach the maximum non-covalent interactions. This work has significantly extended the possibilities of flexible control in self-assembly nanostructures to enable more potential functions for broad applications.

Modifying electrocatalysts nanostructures and tuning their electronic properties through defects-oriented synthetic strategies are essential to improve the oxygen evolution reaction (OER) performance of electrocatalysts. Current synthetic strategies about electrocatalysts mainly target the single or double structural defects, while the researches about the synergistic effect of multiple structural defects are rare. In this work, the ultrathin NiFe layered double hydroxide nanosheets with a holey structure, oxygen vacancies and Ni³⁺ defects on nickel foam (NiFe-LDH-NSs/NF) are prepared by employing a simple and green H₂O₂-assisted etching method. The synergistic effect of the above three defects leads to the exposure of more active sites and significant improvement of the intrinsic activity. The optimized catalyst exhibits an excellent OER performance with an extraordinarily low overpotential of 170 mV at 10 mA·cm⁻² and a small Tafel slope of 39.3 mV·dec⁻¹ in 1 M KOH solution. Density functional theory calculations reveal this OER performance arises from pseudo re-oxidized metal-stable Ni³⁺ near oxygen vacancies (O_vac), which suppresses 3d-e_g of Ni-site and elevates d-band center towards the competitively low electron-transfer barrier. This work provides a new insight to fabricate advanced electrocatalysts for renewable energy conversion technologies.