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At least 127 records · Page 7

Adsorption Properties of Au−Ni Surface Alloys with a Nonstoichiometric Moiré Structure: A Density Functional Theory Study

Due to the large lattice mismatch between gold and nickel, gold–nickel surface alloys can form unique nonstoichiometric overlayer structures characterized by a moiré pattern and subsurface defects. For this work, we performed density functional theory (DFT) calculations to study the adsorption of molecular oxygen, atomic hydrogen, and atomic carbon on a gold–nickel(111) surface alloy with 0.46 monolayer gold randomly distributed in the surface layer. We observed six distinct adsorption structures for molecular oxygen characterized by intramolecular stretching frequencies of <700, 729, 795, 857, 929, and 1004 cm –1 , which describe well the experimentally observed high-resolution electron energy-loss spectra. Surface atomic hydrogen adsorption is associated with adsorbate–surface modes in the ∼1000 cm –1 range, while subsurface hydrogen can have features as low as ∼400 cm –1 . We observed a unique adsorption structure for atomic carbon inside the surface dislocation loop defect, which explains the experimentally observed low carbon-surface mode at ∼340 cm –1 . Our study sheds light on the unique adsorption properties of the gold–nickel surface alloys and helps with rationalizing vibrational frequency experimental studies for this system.

adsorption↗

A Superior Carbonate Electrolyte for Stable Cycling Li Metal Batteries Using High Ni Cathode

Li metal batteries pairing Li metal anode with high-nickel layer structured oxide cathode are a promising energy storage technology to achieve high energy density. To obtain long cycling life for Li metal batteries, the electrolyte plays a pivotal role in stabilizing both the Li metal anode and the high-nickel cathode upon electrochemical cycling. Herein, we report a carbonate electrolyte that enables a Li||LiNi 0.8 Mn 0.1 Co 0.1 O 2 pouch cell to achieve a high gravimetric energy density of 366 Wh/kg and unprecedented cycling stability with 80% capacity retention after 335 cycles. Here, the 19 F quantitative nuclear magnetic resonance spectroscopy and interface characterization demonstrate that FEC and LiDFOB can reduce the consumption rate of each other and the electrolyte, form a robust LiF-rich SEI on Li metal anode, and improve the microstructure integrity of the high-nickel cathode.

25 ENERGY STORAGE↗