Recently, Dan Wang and Ranbo Yu's teams and their collaborators published a research article entitled “Confinement-Induced Enrichment in Hollow Multishelled Structure for High-Efficiency Ammonia Electrosynthesis” in the Journal of the American Chemical Society (Impact Factor: 15.7, CAS Q1, TOP journal). According to the source manuscript, Di Li is the first author, and Dan Wang, Ranbo Yu, Jiawei Wan, and Chang Chen are the corresponding authors.
Electrochemical nitrate reduction is an attractive route for ammonia synthesis because it can proceed under ambient conditions while simultaneously enabling the valorization of nitrate-containing wastewater. Its practical development, however, is often limited by insufficient in situ nitrate enrichment, sluggish interfacial mass transport, and the complexity of multielectron, multiproton reaction pathways.
Article cover
To address these challenges, the team designed a triple-shelled CuO hollow multishelled structure (3s-CuO-HoMS) that behaves as a field-responsive micronanoreactor. The architecture integrates reactant enrichment, spatial confinement, and catalytic conversion within one particle. In situ confocal laser scanning microscopy directly visualized the migration and enrichment of nitrate species inside the stratified cavities, providing compelling evidence that the HoMS architecture actively organizes reactant transport rather than merely serving as a passive support.
The catalyst delivered a Faradaic efficiency of 96.4 ± 0.9% and an ammonia yield of 6316.3 ± 96.1 mmol gcat−1 h−1 at −0.4 V. In situ XAS, Raman, FTIR, and DEMS, together with isotope tracing, revealed the dynamic evolution of the working catalyst and supported a reaction sequence from *NO3 to *NH3 through nitrogen-containing intermediates. This work offers a new design principle for anion-rich micronanoreactors and provides experimental insight into the dynamic catalytic mechanism of electrochemical nitrate reduction.
Representative figure: in situ characterization of catalyst evolution and reaction pathway
This work was supported by the National Key Research and Development Program of China (No. 2024YFA1509400), the National Natural Science Foundation of China (No. 22293043, 92572205, 22505267, 52272097), Shenzhen University 2035 Program for Excellent Research (No. 2024B005), Beijing Natural Science Foundation (No. 2242019) and IPE Project for Frontier Basic Research, China (No. QYJC-2023-08).
Article information Article:Confinement-Induced Enrichment in Hollow Multishelled Structure for High-Efficiency Ammonia Electrosynthesis First author:Di Li Corresponding authors:Dan Wang, Ranbo Yu, Jiawei Wan, and Chang Chen Journal:Journal of the American Chemical Society DOI:10.1021/jacs.6c01046 |