Electrocatalytic conversion of CO into value-added products offers a new paradigm for a sustainable carbon economy. For active CO electrolysis, the single-atom Ni catalyst has been proposed as promising from experiments, but an idealized Ni-N site shows an unfavorable energetics from theory, leading to many debates on the chemical nature responsible for high activity. To resolve this conundrum, here we investigated CO electrolysis of Ni sites with well-defined coordination, tetraphenylporphyrin (N-TPP) and 21-oxatetraphenylporphyrin (NO-TPP).
View Article and Find Full Text PDFCarbon monoxide is widely known to poison Pt during heterogeneous catalysis owing to its strong donor-acceptor binding ability. Herein, we report a counterintuitive phenomenon of this general paradigm when the size of Pt decreases to an atomic level, namely, the CO-promoting Pt electrocatalysis toward hydrogen evolution reactions (HER). Compared to pristine atomic Pt catalyst, reduction current on a CO-modified catalyst increases significantly.
View Article and Find Full Text PDFCatalysis is a key technology for the synthesis of renewable fuels through electrochemical reduction of CO2 . However, successful CO2 reduction still suffers from the lack of affordable catalyst design and understanding the factors governing catalysis. Herein, we demonstrate that the CO2 conversion selectivity on Sn (or SnOx /Sn) electrodes is correlated to the native oxygen content at the subsurface.
View Article and Find Full Text PDFN-doped carbon materials are considered as next-generation oxygen reduction reaction (ORR) catalysts for fuel cells due to their prolonged stability and low cost. However, the underlying mechanism of these catalysts has been only insufficiently identified, preventing the rational design of high-performing catalysts. Here, we show that the first electron is transferred into O2 molecules at the outer Helmholtz plane (ET-OHP) over a long range.
View Article and Find Full Text PDFPhosphorus and/or sulfur are additionally doped into N-doped carbon (NDC) using phosphoric acid and cysteine. The resulting catalysts demonstrate excellent oxygen reduction activities coupled with high stabilities in acidic media. Specially, additional S-doping in NDC reveals nearly 2.
View Article and Find Full Text PDF