Electrochemical energy storage devices are ubiquitous for personal electronics, electric vehicles, smart grids, and future clean energy demand. SCs are EES devices with excellent power density and superior cycling ability. Herein, we focused on the fabrication and DFT calculations of Na₃-δ-MnO₂ nanocomposite, which has layered MnO₂ redox-active sites, supported on carbon cloth. MnO₂ has two-dimensional diffusion channels and is not labile to structural changes during intercalation; therefore, it is considered the best substrate for intercalation. Cation pre-intercalation has proven to be an effective way of increasing inter-layered spacing, optimizing the crystal structure, and improving the relevant electrochemical behavior of asymmetric aqueous supercapacitors. We successfully established Na⁺ pre-intercalated δ-MnO₂ nanosheets on carbon cloth via one-pot hydrothermal synthesis. As a cathode, our prepared material exhibited an extended potential window of 0–1.4 V with a remarkable specific capacitance of 546 F g⁻¹(300 F g⁻¹ at 50 A g⁻¹). Moreover, when this cathode was accompanied by an N-AC anode in an asymmetric aqueous supercapacitor, it illustrated exceptional performance (64 Wh kg⁻¹ at a power density of 1225 W kg⁻¹) and incomparable potential window of 2.4 V and 83% capacitance retention over 10,000 cycles with a great Columbic efficiency.

Herein, we report a protocol for highly efficient hypervalent iodine (III) mediated, group-assisted purification (GAP) method for the regioselectivities and stereoselective aminochlorination of electron-deficient olefins. A series of vicinal chloramines with multifunctionalities were acquired in moderate to excellent yields (45–94%), by merely mixing the GAP auxiliary-anchored substrates with dichloramine T and tosylamide as chlorine/nitrogen sources and iodobenzene diacetate as a catalyst. The vicinal chloramines were obtained without any column chromatographic purification and recrystallization simply by washing the reaction mixture with a minimum amount of common inexpensive solvents and thus avoiding wastage of silica, solvents, time, and labor. The GAP auxiliary is recyclable and reusable. This strategy is easy to handle, cost-effective, greener, sustainable, environmentally benign, and mostly suitable for the syntheses of vicinal haloamines from various electron-deficient alkenes.

Simultaneously regulating charge carrier dynamics and catalytic selectivity remains a critical challenge in photocatalytic CO ₂ reduction. Here, we report a copper (II) phthalocyanine/oxygen‐vacancy‐rich (CuPc/CeO ₂ ) S‐scheme heterojunction featuring atomically dispersed Cu–N ₄ sites. Ultraviolet photoelectron spectroscopy establishes a 0.24 eV work function difference between CeO ₂ and CuPc, generating a built‐in electric field that drives S‐scheme charge transfer. X‐ray photoelectron spectroscopy confirms oxygen vacancies in CeO ₂ (evidenced by Ce ³⁺ states), enabling the energetic alignment that spatially separates reductive electrons (−1.05 V vs. NHE) at molecular Cu sites from oxidative holes (+2.44 V) in CeO ₂ . Time‐resolved photoluminescence spectroscopy confirmed that the reduction in carrier lifetime (from 7.42 to 6.57 ns) corroborates an efficient charge separation process. In situ diffuse reflectance infrared Fourier‐transform spectroscopy demonstrates that the Cu–N ₄ centers preferentially stabilize the *COOH intermediate while facilitating rapid CO desorption from Cu(I) sites, thereby directing selective two‐electron reduction and suppressing over‐reduction to CH ₄ . The optimized 20CuPc/CeO ₂ catalyst achieves a CO generation rate of 90.23 μmol g ⁻¹ h ⁻¹ —representing a 16.96‐fold enhancement over pristine CeO ₂ —with 92.2% selectivity for CO versus CH ₄ , and maintains robust stability over five consecutive photocatalytic cycles. This work establishes a unified design strategy integrating defect‐engineered S‐scheme charge separation with single‐atom molecular catalysis to achieve selective solar‐driven CO ₂ ‐to‐CO conversion.