Fore lectrocatalysts for the hydrogen evolution reaction (HER), encapsulating transition metal phosphides (TMPs) into nitrogen-doped carbon materials has been known as an effective strategy to elevate the activity and stability.Y et still, it remains unclear how the TMPs work synergistically with the N-doped support, and which Nc onfiguration (pyridinic N, pyrrolic N, or graphitic N) contributes predominantly to the synergy.H ere we present aH ER electrocatalyst (denoted as MoP@NCHSs) comprising MoP nanoparticles encapsulated in N-doped carbon hollows pheres,w hich displays excellent activity and stability for HER in alkaline media. Results of experimental investigations and theoretical calculations indicate that the synergy between MoP and the pyridinic Ncan most effectively promote the HER in alkaline media.
The development of highly active and stable bifunctional noble-metal-based electrocatalysts for the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) is a crucial goal for clean and renewable energy, which still remains challenging. Herein, we report an efficient and stable catalyst comprising a Co single atom incorporated in an RuO 2 sphere for HER and OER, in which the Co single atom in the RuO 2 sphere was confirmed by XAS, AC-STEM, and DFT. This tailoring strategy uses a Co single atom to modify the electronic structures of the surrounding Ru atoms and thereby remarkably elevates the electrocatalytic activities. The catalyst requires ultralow overpotentials, 45 mV for HER and 200 mV for OER, to deliver a current density of 10 mA cm À 2 . The theoretical calculations reveal that the energy barriers for HER and OER are lowered after incorporation of a cobalt single atom.
High‐performance, fully atomically dispersed single‐atom catalysts (SACs) are promising candidates for next‐generation industrial catalysts. However, it remains a great challenge to avoid the aggregation of isolated atoms into nanoparticles during the preparation and application of SACs. Here, the evolution of Pd species is investigated on different crystal facets of CeO2, and vastly different behaviors on the single‐atomic dispersion of surface Pd atoms are surprisingly discovered. In situ X‐ray photoelectron spectroscopy (XPS), in situ near‐ambient‐pressure‐XPS (NAP‐XPS), in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and X‐ray absorption spectroscopy (XAS) reveal that, in a reducing atmosphere, more oxygen vacancies are generated on the (100) facet of CeO2, and Pd atoms can be trapped and thus feature atomic dispersion; by contrast, on the CeO2 (111) facet, Pd atoms will readily aggregate into clusters (Pdn). Furthermore, Pd1/CeO2(100) gives a high selectivity of 90.3% for the catalytic N‐alkylation reaction, which is 2.8 times higher than that for Pdn/CeO2(111). This direct evidence demonstrates the crucial role of crystal‐facet effects in the preparation of metal‐atom‐on‐metal‐oxide SACs. This work thus opens an avenue for the rational design and targeted synthesis of ultrastable and sinter‐resistant SACs.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.