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Lithium‐ion batteries (LIBs) with conventional carbonate‐based electrolytes suffer from safety concerns in large‐scale applications. Phosphates feature high flame retardancy but are incompatible with graphite anode due to their inability to form a passivated solid electrolyte interphase (SEI). Herein, we report a monofluorinated co‐solvent, diethyl fluoridophosphate (DEFP), featuring a unique P−F bond that allows a trade‐off between safety and electrochemical performance in LIBs. The P−F bond in DEFP weakens ion‐dipole interactions with Li+ ions, lowering the desolvation barrier, and simultaneously reduces the lowest unoccupied molecular orbital (LUMO) of DEFP, promoting the formation of a robust and inorganic‐rich SEI. Additionally, DEFP exhibits improved thermal stability due to both robust SEI and the inherent flame‐retardant properties of the P−F bond. Consequently, the optimized DEFP‐based electrolyte exhibits improved cyclability and rate capacity in LiNi0.8Co0.1Mn0.1O2||graphite full cells compared with triethyl phosphate‐based electrolytes and commercial carbonate electrolytes. Even at a low E/C ratio of 3.45 g Ah−1, the 1.16 Ah NCM811||Gr pouch cells achieve a high capacity retention of 94.2 % after 200 cycles. This work provides a promising approach to decouple phosphate safety and graphite compatibility, paving the way for safer and high‐performance lithium‐ion batteries. [ABSTRACT FROM AUTHOR]

Transformation of lignin to syngas can turn waste into treasure yet remains a tremendous challenge because of its naturally evolved stubborn structure. In this work, light‐driven reforming of natural lignin in water for green syngas production is explored using Pt‐decorated InGaN nanowires. The spectroscopic characterizations, isotope, and model compound experiments, as well as density function theory calculation, disclose that among a variety of groups including aromatic ring, −OH, −OCH3, −C3H7 with complex chemical bonds of O−H, C−H, C−C, C−O, etc., InGaN nanowires are cooperative with Pt for preferably breaking the C−O bond of the rich O−CH3 group in lignin to liberating ⋅CH3 by photogenerated holes with a minimum dissociation energy of 2.33 eV. Syngas are subsequently yielded from the continuous evolution of ⋅CH3 and ⋅OH from photocatalytic reforming of lignin in water. Together with the superior optoelectronic attributes of Pt‐decorated InGaN nanowires, the evolution rate of syngas approaches 43.4 mol ⋅ g−1 ⋅ h−1 with tunable H2/CO ratios and a remarkable turnover number (TON) of 150, 543 mol syngas per mol Pt. Notably, the architecture demonstrates a high light efficiency of 12.1 % for syngas generation under focused light without any extra thermal input. Outdoor test ascertains the viability of producing syngas with the only inputs of natural lignin, water, and sunlight, thus presenting a low‐carbon route for synthesizing transportation fuels and value‐added chemicals. [ABSTRACT FROM AUTHOR]

Light‐driven hydrogen production from biomass derivatives offers a path towards carbon neutrality. It is often however operated with the limitations of sluggish kinetics and severe coking. Herein, a disruptive air‐promoted strategy is explored for efficient and durable light‐driven hydrogen production from ethanol over a core/shell Cr2O3@GaN nanoarchitecture. The correlative computational and experimental investigations show ethanol is energetically favorable to be adsorbed on the Cr2O3@GaN interface, followed by dehydrogenation toward acetaldehyde and protons by photoexcited holes. The released protons are then consumed for H2 evolution by photogenerated electrons. Afterward, O2 can be evolved into active oxygen species and promote the deprotonation and C−C cleavage of the key C2 intermediate, thus significantly lowering the reaction energy barrier of hydrogen evolution and removing the carbon residual with inhibited overoxidation. Consequently, hydrogen is produced at a high rate of 76.9 mole H2 per gram Cr2O3@GaN per hour by only feeding ethanol, air, and light, leading to the achievement of a turnover number of 266,943,000 mole H2 per mole Cr2O3 over a long‐term operation of 180 hours. Notably, an unprecedented light‐to‐hydrogen efficiency of 17.6 % is achieved under concentrated light illumination. The simultaneous generation of aldehyde from ethanol dehydrogenation enables the process more economically promising. [ABSTRACT FROM AUTHOR]