Photochemical conversion of CO₂ into high-value C₂₊ products is difficult to achieve due to the energetic and mechanistic challenges in forming multiple C-C bonds. Herein, an efficient photocatalyst for the conversion of CO₂ into C₃H₈ is prepared by implanting Cu single atoms on Ti_0.91O₂ atomically-thin single layers. Cu single atoms promote the formation of neighbouring oxygen vacancies (V_Os) in Ti_0.91O₂ matrix. These oxygen vacancies modulate the electronic coupling interaction between Cu atoms and adjacent Ti atoms to form a unique Cu-Ti-V_O unit in Ti_0.91O₂ matrix. A high electron-based selectivity of 64.8% for C₃H₈ (product-based selectivity of 32.4%), and 86.2% for total C₂₊ hydrocarbons (product-based selectivity of 50.2%) are achieved. Theoretical calculations suggest that Cu-Ti-V_O unit may stabilize the key *CHOCO and *CH₂OCOCO intermediates and reduce their energy levels, tuning both C₁-C₁ and C₁-C₂ couplings into thermodynamically-favourable exothermal processes. Tandem catalysis mechanism and potential reaction pathway are tentatively proposed for C₃H₈ formation, involving an overall (20e⁻ – 20H⁺) reduction and coupling of three CO₂ molecules at room temperature.

Artificial photosynthesis, light-driving CO₂ conversion into hydrocarbon fuels, is a promising strategy to synchronously overcome global warming and energy-supply issues. The quaternary AgInP₂S₆ atomic layer with the thickness of ~ 0.70 nm were successfully synthesized through facile ultrasonic exfoliation of the corresponding bulk crystal. The sulfur defect engineering on this atomic layer through a H₂O₂ etching treatment can excitingly change the CO₂ photoreduction reaction pathway to steer dominant generation of ethene with the yield-based selectivity reaching ~73% and the electron-based selectivity as high as ~89%. Both DFT calculation and in-situ FTIR spectra demonstrate that as the introduction of S vacancies in AgInP₂S₆ causes the charge accumulation on the Ag atoms near the S vacancies, the exposed Ag sites can thus effectively capture the forming *CO molecules. It makes the catalyst surface enrich with key reaction intermediates to lower the C-C binding coupling barrier, which facilitates the production of ethene.

Solid-state polymer electrolytes (SPEs) with superior self-healing capacity are urgently required for next-generation flexible energy storage devices. Herein, a highly stretchable (extensibility > 4000% and stress > 130 kPa), non-flammable and notch-insensitive intrinsic self-healing solid-state polymer electrolyte (SHSPE) was prepared based on the combination of a poly(HFBM-co-SBMA) network, imidazole-based ionic liquid (EMI–TFSI) and LiTFSI. The incorporation of the imidazole cation and fluorine atom contributed to the formation of supramolecular bonds (ion–dipole interactions) inside the electrolyte framework, thus endowing SHSPE with prominent self-healing ability (recovery time < 60 min, 25 °C). Moreover, the density functional theory (DFT) calculations indicated that the large electrostatic attraction of SO₃ ⁻ towards Li⁺ liberated it from trapping in the ionic reservoir of TFSI⁻ and EMI⁺, thereby resulting in a superior t_Li⁺ (0.37). The electrochemical window of SHSPE achieved was 4.9 V vs. Li⁺/Li, which well satisfies the demand for safe lithium batteries. The optimized SHSPE3 presented excellent interfacial compatible property with a lithium electrode and record adhesion strength (weight loading > 200 g). The as-assembled Li/SHSPE3/LiFePO₄ battery delivered a high discharge capacity of 144.8 mA h g⁻¹ at 0.2C, and its capacity retention ratio reached 82% after 100 cycles with a coulombic efficiency of 97%. In particular, the mechanical properties and conductivity of SHSPE3 could fully recover after repeated damage, conferring the derived soft-pack battery excellent anti-fatigue capability. The use of intrinsic self-healing principles in the field of SPEs provides new insight for developing reliable and safe flexible electronic devices.