Platinum-nanoparticle-based catalysts are widely used in many important chemical processes and automobile industries. Downsizing catalyst nanoparticles to single atoms is highly desirable to maximize their use efficiency, however, very challenging. Here we report a practical synthesis for isolated single Pt atoms anchored to graphene nanosheet using the atomic layer deposition (ALD) technique. ALD offers the capability of precise control of catalyst size span from single atom, subnanometer cluster to nanoparticle. The single-atom catalysts exhibit significantly improved catalytic activity (up to 10 times) over that of the state-of-the-art commercial Pt/C catalyst. X-ray absorption fine structure (XAFS) analyses reveal that the low-coordination and partially unoccupied densities of states of 5d orbital of Pt atoms are responsible for the excellent performance. This work is anticipated to form the basis for the exploration of a next generation of highly efficient single-atom catalysts for various applications.
Electrochemical CO2 reduction can produce valuable products with high energy densities but the process is plagued by poor selectivities and low yields. Propanol represents a challenging product to obtain due to the complicated C3 forming mechanism that requires both stabilization of *C2 intermediates and subsequent C1–C2 coupling. Herein, density function theory calculations revealed that double sulfur vacancies formed on hexagonal copper sulfide can feature as efficient electrocatalytic centers for stabilizing both CO* and OCCO* dimer, and further CO–OCCO coupling to form C3 species, which cannot be realized on CuS with single or no sulfur vacancies. The double sulfur vacancies were then experimentally synthesized by an electrochemical lithium tuning strategy, during which the density of sulfur vacancies was well-tuned by the charge/discharge cycle number. The double sulfur vacancy-rich CuS catalyst exhibited a Faradaic efficiency toward n-propanol of 15.4 ± 1% at −1.05 V versus reversible hydrogen electrode in H-cells, and a high partial current density of 9.9 mA cm−2 at −0.85 V in flow-cells, comparable to the best reported electrochemical CO2 reduction toward n-propanol. Our work suggests an attractive approach to create anion vacancy pairs as catalytic centers for multi-carbon-products.
Sandwiched structures consisting of carbon coated SnO2 nanorod grafted on graphene have been synthesized based on a seed assisted hydrothermal growth to form graphene supported SnO2 nanorods, followed by a nanocarbon coating. As a potential anode for high power and energy applications, the hierarchical nanostructures exhibit a greatly enhanced synergic effect with an extremely high lithium storage capability of up to 1419 mA h g−1 benefiting from the advanced structural features.