Assembly-line synergistic catalysis in isomorphic substituted Co3O4 nanocomposite for enhanced N2O decomposition

doi:10.1016/S1872-2067(26)65175-3

Abstract

Abstract:

Nanoscale assembly-line catalysis is a novel avenue for reactions with multiple rate-determining steps. The regional coexistence of different elements in nanocomposites with adjacent heterometallic coordination can construct substructures compatible with multifunctional sites, resulting in synergistic catalysis. Herein, a novel nanocomposite with affluent Ca-O-Co-O_v-Zr micro-integrated stations (MIS) is developed through an isomorphic substitution strategy to promote the spatiotemporally ordered N-O adsorption and mitigate kinetic limitation of O transportation/desorption through an assembly-line catalytic perspective during N₂O decomposition. The optimized CoCa₆Zr₉ can achieve T₉₀ of N₂O decomposition at 355 °C and stably run for more than 100 h. This superior performance is mainly attributed to a bidirectional promotion mechanism via both “Ca-e^--Co” electronic chain in Ca-O-Co (workshop 1) and O vacancy electronic pump in “Co-O_v-Zr” (workshop 2), which promotes the formation of electron-rich Co²⁺-O_v cooperative sites (namly, the MIS), accelerating cleavage of N-O bond (Primary Step i). Meanwhile, the cooperative of atomic-regulated electronic and redox inducers can adjust the Co-O polarity to maintain the Co²⁺ valence state, weaken the Co-O bond and enhance active oxygen mobility, thus refreshing its active sites for assembly-line catalytic cycles instantly and persistently (Primary Step ii). This work establishes an effective insight for rationally assembling cooperative active sites in assembly-line inspired substructures, which is essential for advancing the research on the coordination of multiple reaction steps in complex catalytic reactions.

Key words: Assembly-line catalysis, Isomorphic substituted substructure, Nanocomposite, Bidirectional promotion, N₂O decomposition

Lingji Liu, Xiaosheng Yu, Zhou Chen, Xueqing Hai, Yongzhao Wang, Changzhen Wang, Tiancun Xiao. Assembly-line synergistic catalysis in isomorphic substituted Co₃O₄ nanocomposite for enhanced N₂O decomposition[J]. Chinese Journal of Catalysis, 2026, 89: 430-443.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65175-3

https://www.cjcatal.com/EN/Y2026/V89/I10/430

Figures/Tables 5

Fig. 1. Schematic synthetic procedures and structural characterizations of the nanocomposites. (a) Schematic illustration for the preparation of the CoCaZr nanocomposites. HR-TEM (b), HAADF-STEM images and EDX element mappings (c), high-resolution atomic contrast imaging (d) of the CoCa6Zr9 from position I in (b). HR-TEM and corresponding GPA images of CoCa6Zr9 from position II (e) and reference Co3O4 with strain tensor maps (f) in xy direction (εxy). (e1) Schematic representation of the regional balance of tensile and compressive lattice strains. (g) XRD patterns in rietveld refinement of Co3O4 and CoCa6Zr9. The Fourier transform spectra of k2-Co K-edge EXAFS (h), Zr 3d XPS (i) and Ca 2p XPS (j) spectra for Co3O4, CoCa6Zr9 and Co/Ca6Zr9.

Fig. 2. Catalytic performance evaluation. N2O decomposition activity (a) and Arrhenius plots (b) for the decomposition of N2O over Co3O4, CoCa6Zr9 and Co/Ca6Zr9. N2O decomposition activity (c), Arrhenius plots (d) for the decomposition of N2O and reaction rates (e) at 300 and 350 °C over CoCaxZry nanocomposites. Reaction conditions: 1000 ppm N2O balanced with Ar, GHSV = 10000 h-1. (f) The schematic of structural properties of the Ca-O-Co-Ov-Zr substructure. (g) Stability test at 400 °C over CoCa6Zr9, Co3O4, Co/Ca6Zr9 catalysts and 355 °C over CoCa6Zr9 nanocomposite. (h) T90 and stability performance of CoCa6Zr9 and their comparison with the reported Co-based catalysts (refer to Table S4 for details), and (i) Test of impurities resistance over CoCa6Zr9 nanocomposite.

Fig. 3. Promotion factors analysis. The Co K-edge XANES spectra (a), H2-TPR profiles (b), CO2-TPD profiles (c), EPR spectra (d), O 1s XPS spectra (e), and O2-TPD profiles (f) of CoCaxZry nanocomposites. (g) The linear fitting relationship between the reaction rate at 300 °C and Co2+/Co3+ from Co XPS spectra, Oads/(Oads+Olat) from O XPS spectra, the Co2+ maintenance ability (reduction temperature of peak-2 in H2-TPR), the basic ability (desorption temperature of peak-I in CO2-TPD). (h) Possible bidirectional promotion mechanism on the surface of CoCaxZry nanocomposites.

Fig. 4. Theoretical calculation. N2O adsorption configurations of Co-O-Co (311) (a), Ca-O-Co-O-Zr (311) (b), and Ca-O-Co-Ov-Zr (311) (c). (d) The PDOS of the Co atoms on the Co-O-Co, Ca-O-Co-O-Zr, and Ca-O-Co-Ov-Zr; the black dashed line implies the Ef energy. The differential charge density diagram of Co-O-Co (e), Ca-O-Co-O-Zr (f), and Ca-O-Co-Ov-Zr (g), in which the cyan and yellow regions stand for the depletion and accumulation of charges, respectively. (h) Schematic illustration of electron transfer between Ca-O-Co-Ov-Zr and N2O. (i) The PDOS of the N2O molecule is adsorbed on the Co-O-Co, Ca-O-Co-O-Zr, and Ca-O-Co-Ov-Zr. (j) Schematic illustration of the orbital interactions between Co 3d and N2O 3π*. (k) Optimized structures and calculated transition state (TS) of N2O decomposition over the Co-O-Co (311) and Ca-O-Co-Ov-Zr (311) surface.

Fig. 5. N2O decomposition mechanism. O XPS spectra (a) and Co XPS (b) spectra of results of the fresh (dash line)/spent (solid line) CoCa6Zr9, Co3O4, and Co/Ca6Zr9 catalysts. (c) Concentration variation ratio of Oads/(Oads+Olat), and Co2+/(Co2+ + Co3+) before and after the reaction of the CoCa6Zr9, Co3O4, and Co/Ca6Zr9. (d) In situ FT-IR spectra of the CoCa6Zr9 catalyst recorded at 50 °C upon passing 1000 ppm of N2O. In-situ FT-IR spectra obtained during catalytic decomposition of N2O (1000 ppm) over CoCa6Zr9 (e) and Co3O4 (f) at varied temperatures. (g) Reaction stability mechanism in N2O decomposition over CoCa6Zr9 nanocomposite. (h) Schematic illustration of the assembly-line catalysis mechanism vs traditional catalysis.

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Assembly-line synergistic catalysis in isomorphic substituted Co₃O₄ nanocomposite for enhanced N₂O decomposition

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