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Architecting Cobalt-Centered 2D Sandwich-Type Polyoxometalate Frameworks for Selective Electrocatalytic Nitrate
Hui Luo1, Xinming Wang1, Qiushuang Jiang1
1Key Laboratory of Green Chemical Engineering and Technology of College of Heilongjiang Province, School of Materials Science and Chemical Engineering, Harbin University of Science and Technology, Harbin 150040, P. R. China.
None:
Developing efficient electrocatalysts for neutral-media nitrate reduction (NO3-RR) is crucial for simultaneous nitrate remediation and sustainable ammonia (NH3) synthesis, yet hindered by sluggish reaction kinetics. Herein, we designed and synthesized four novel two-dimensional (2D) cobalt-centered hourglass-shaped [P4Mo6VO31]12--based crystalline materials via the hydrothermal method: (H2bimb)2[Co3{Mo6O15(HPO4)3(PO4)}2]·7H2O (1), (H2bimb)2[Co3{Mo6O15(HPO4)3(PO4)}2]·16H2O (2), [{Co(Hbimb)2}2][{Co(H2O)2}Co{Mo6O15(HPO4)2(PO4)2}2]·10H2O (3), and (H2bimb)2[Co(Hbimb)2][{Co(H2O)2}2Co{Mo6O15(HPO4)2(PO4)2}2]·18H2O (4) (bimb = 1,3-bis(1H-imidazol-1-yl)benzene), featuring tunable hourglass-type [P4Mo6VO31]12- clusters. The experimental results showed that compounds 1-4 all exhibited better NO3-RR performance, among which compound 4 exhibited excellent stability and outstanding redox activity performance with a Faradaic efficiency of 89.65% at -0.7 V (versus reversible hydrogen electrode) and an ammonia synthesis rate of 8.97 mg h-1 mgcat-1. This work extends the application of e-NO3-RR catalysts based on polymetallic oxides and opens up innovative pathways for sustainable ammonia synthesis through molecular-level structure modulation.
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