Atomic Interface‐Exciting Catalysis on Cobalt Nitride‐Oxide for Accelerating Hydrogen Generation

Abstract

The rational design of the interface structure between nitride and oxide using the same metallic element and correlating the interfacial active center with a determined catalytic mechanism remain challenging. Herein, a Co4N‐Co3O4 interface structure is designed to determine the effect of interfacial active centers on hydrogen generation from ammonia borane. An unparalleled catalytic activity toward H2 production with a turnover frequency up to 79 min−1 is achieved on Co4N‐Co3O4@C catalyst for ten recycles. Experimental analyses and theoretical simulation suggest that the atomic interface‐exciting effect (AieE) is responsible for the high catalytic activity. The Co4N‐Co3O4 interface facilitates the targeted adsorption and activation of NH3BH3 and H2O molecules to generate H* and H2. The two active centers of Co(N)* and Co(O)* at the Co4N‐Co3O4 interface activate NH3BH3 and H2O, respectively. This proof‐of‐concept research on AieE provides important insights regarding the design of heterogeneous catalysts and promotes the development of the nature and regulation of energy chemical conversion.

“On–Off” Control for On-Demand H2 Release upon Dimethylamineborane Hydrolysis over Ru0.8Ni0.2/MoS2 Nanohybrids

“…In addition, the catalytic activity of Ru 0.8 Ni 0.2 /MoS 2 with that of other reported catalysts in dimethylamineborane hydrolysis was further summarized and is compared in Table . − The result showed that as-obtained Ru 0.8 Ni 0.2 /MoS 2 exhibited the excellent catalytic performance in H 2 release upon dimethylamineborane hydrolysis, with 7199 mol (H 2 )·mol cat –1 ·h –1 at 30 °C under 2 M NaOH, which exceeds almost other reported catalysts. − …”

Recent Advances and Perspectives on Supported Catalysts for Heterogeneous Hydrogen Production from Ammonia Borane

“…Reproduced with permission. [ 149 ] Copyright 2022, Wiley‐VCH. d,e) Comprehensive morphology characterization of g‐C 3 N 4 .…”

“…Subsequently, Li designed Co (N) * and Co (O) * double active sites and combined the double active sites with AB and H 2 O molecules to analyze the reaction path (Figure 31e). [ 149 ] The specific reaction path is as follows: $$$$\begin{equation}{\rm{NH}}_3{\rm{BH}}_3 + {\rm{Co}}_{({\rm{N}})}^* = {\rm{NH}}_3{\rm{BH}}_2 - {\rm{Co}}_{({\rm{N}})}^* + {{\rm{H}}}^*\end{equation}$$$$ $$$$\begin{equation}{{\rm{H}}}_2{\rm{O}} + {\rm{Co}}_{({\rm{O}})}^* = {\rm{HO}} - {\rm{Co}}_{({\rm{O}})}^* + {{\rm{H}}}^*\end{equation}$$$$ $$$$\begin{eqnarray} && {\rm{NH}}_3{\rm{BH}}_2 - {\rm{Co}}_{({\rm{N}})}^* + {\rm{ H}}^* + {\rm{HO}} - {\rm{Co}}_{({\rm{O}})}^* + {{\rm{H}}}^* \nonumber \\ && \quad = {\rm{HO}} - {\rm{Co}}_{({\rm{O}})}^* + {\rm{NH}}_3{\rm{BH}}_2{\rm{OH}} - {\rm{Co}}_{({\rm{N}})}^* + {{\rm{H}}}_2 \uparrow \end{eqnarray}$$$$ $$…”

“…The stabil-ity of the Co 4 N-Co 3 O 4 interface structure was verified by theoretical simulation, and the atomic interface-exciting effect (AieE) was the main reason for its high catalytic activity. [149] Li et al prepared monodisperse Ni NPs with controllable sizes using a simple method and fixed them on graphitized carbon nitride (g-C 3 N 4 ) nanosheets by self-assembly (Figure 16d,e). The Ni/g-C 3 N 4 composite catalyst showed good photocatalytic activity for hydrolytic [109] Copyright 2020, Elsevier.…”

Bimetallic PtNi Nanoclusters Supported on Carbon Nanospheres as Catalysts for H2 Production from Dimethylamineborane Hydrolysis

“…It is also found that catalytic activity of the Pt 0.7 Ni 0.3 /CNS nanohybrid had been greatly enhanced, from 4955 to 16,607 mol (H 2 )·mol cat –1 ·h –1 by aqueous alkali. This is probably because the electron density of Pt atoms was enriched by the coordination of OH – anion, which is in favor of the breaking of a water O – H bond. − …”