Compressive surface strains have been necessary to boost oxygen reduction reaction (ORR) activity in core/shell M/platinum (Pt) catalysts (where M can be nickel, cobalt, or iron). We report on a class of platinum-lead/platinum (PtPb/Pt) core/shell nanoplate catalysts that exhibit large biaxial strains. The stable Pt (110) facets of the nanoplates have high ORR specific and mass activities that reach 7.8 milliampere (mA) per centimeter squared and 4.3 ampere per milligram of platinum at 0.9 volts versus the reversible hydrogen electrode (RHE), respectively. Density functional theory calculations reveal that the edge-Pt and top (bottom)-Pt (110) facets undergo large tensile strains that help optimize the Pt-O bond strength. The intermetallic core and uniform four layers of Pt shell of the PtPb/Pt nanoplates appear to underlie the high endurance of these catalysts, which can undergo 50,000 voltage cycles with negligible activity decay and no apparent structure and composition changes.
The development of active, acid-stable and low-cost electrocatalysts for oxygen evolution reaction is urgent and challenging. Herein we report an Iridium-free and low ruthenium-content oxide material (Cr0.6Ru0.4O2) derived from metal-organic framework with remarkable oxygen evolution reaction performance in acidic condition. It shows a record low overpotential of 178 mV at 10 mA cm−2 and maintains the excellent performance throughout the 10 h chronopotentiometry test at a constant current of 10 mA cm−2 in 0.5 M H2SO4 solution. Density functional theory calculations further revealed the intrinsic mechanism for the exceptional oxygen evolution reaction performance, highlighting the influence of chromium promoter on the enhancement in both activity and stability.
All-inorganic lead halide perovskites demonstrate improved thermal stability over the organic-inorganic halide perovskites, but the cubic α-CsPbI with the most appropriate bandgap for light harvesting is not structurally stable at room temperature and spontaneously transforms into the undesired orthorhombic δ-CsPbI. Here, we present a new member of black-phase thin films of all-inorganic perovskites for high-efficiency photovoltaics, the orthorhombic γ-CsPbI thin films with intrinsic thermodynamic stability and ideal electronic structure. Exempt from introducing organic ligands or incorporating mixed cations/anions into the crystal lattice, we stabilize the γ-CsPbI thin films by a simple solution process in which a small amount of HO manipulates the size-dependent phase formation through a proton transfer reaction. Theoretical calculations coupled with experiments show that γ-CsPbI with a lower surface free energy becomes thermodynamically preferred over δ-CsPbI at surface areas greater than 8600 m/mol and exhibits comparable optoelectronic properties to α-CsPbI. Consequently, γ-CsPbI-based solar cells display a highly reproducible efficiency of 11.3%, among the highest records for CsPbI thin-film solar cells, with robust stability in ambient atmosphere for months and continuous operating conditions for hours. Our study provides a novel and fundamental perspective to overcome the Achilles' heel of the inorganic lead iodide perovskite and opens it up for high-performance optoelectronic devices.
The grand challenge in the development of atomically dispersed metallic catalysts is their low metal-atom loading density, uncontrollable localization and ambiguous interactions with supports, posing difficulty in maximizing their catalytic performance. Here, we achieve an interface catalyst consisting of atomic cobalt array covalently bound to distorted 1T MoS2 nanosheets (SA Co-D 1T MoS2). The phase of MoS2 transforming from 2H to D-1T, induced by strain from lattice mismatch and formation of Co-S covalent bond between Co and MoS2 during the assembly, is found to be essential to form the highly active single-atom array catalyst. SA Co-D 1T MoS2 achieves Pt-like activity toward HER and high long-term stability. Active-site blocking experiment together with density functional theory (DFT) calculations reveal that the superior catalytic behaviour is associated with an ensemble effect via the synergy of Co adatom and S of the D-1T MoS2 support by tuning hydrogen binding mode at the interface.
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