The development of high-performance oxygen carriers (OCs) for chemical looping dry reforming of methane (CLDRM) is often hindered by the sluggish kinetics of C–H bond activation and the susceptibility to carbon deposition. Herein, we report that A-site Y doping in LaFeO3 (La0.9Y0.1FeO3) perovskite significantly enhances methane reactivity, achieving a CH4 conversion of 93–98% and a syngas yield nearly twice that of pristine LaFeO3, alongside an ideal H2/CO ratio (1.97–1.99) and stable performance at 900 °C over 30 CH4/CO2 redox cycles. Experimental and DFT analysis reveal a two-stage “active-site relay” activation mechanism. Initially, Y doping in the perovskite induces lattice distortion and enlarges Fe–O–Fe bond angles, which boosts lattice oxygen mobility and facilitates surface C–H bond cleavage. Subsequently, deep reduction triggers the in situ exsolution of metallic Fe0 nanoparticles, serving as highly active secondary centers for CH4 dissociation. The synergistic effect between exsolved Fe0 and the Y-doped perovskite with high mobility of lattice oxygen ensures rapid coke elimination, thereby enabling good cyclic stability. The strategy of the “active-site relay” can provide principles for rationally designing advanced OCs.
Chemical looping reforming of CH4 coupled with CO2 splitting (CLRCS) is an attractive technology that enables covalorization of CO2 and CH4 to high- value syngas. In CLRCS, oxygen carriers shuttle oxygen from CO2 to CH4, enabling selective methane partial oxidation and CO2 splitting. However, rational optimization of p...
Developing the efficient catalysts with both high 2e- selectivity and stability remains challenging for on-site hydrogen peroxide (H2O2) synthesis. Perovskite oxides possess dense isolated active sites to convert O2 into H2O2, yet their intrinsic structural instability is also equally noteworthy. In this work, one kind...
Jian-Qi Zhang, Yan-Zong Huang, Ya-Jing Di et al.· Small· 0 citations
La1-xSrxFeO3 (0 ≤ x ≤ 1) perovskite oxygen carriers (OCs) were evaluated for dry reforming of methane (DRM) at 900°C under co-feed and chemical-looping (CL-DRM) configurations. Sr substitution decreased CH4/CO2 conversions in co-feed DRM, indicating suppressed intrinsic catalytic activity. In contrast, CL-DRM enhanced...
Ganesh Jabotra, Pradeep Kumar Yadav, L. Stievano et al.· Chemistry· 0 citations
Dry reforming of methane (DRM) is a sustainable method to produce valuable syngas from two important greenhouse gases, CH4 and CO2. Traditional thermal DRM requires high temperatures, resulting in high carbon deposition, while photothermal catalysis reduces the energy barrier by using solar light and creates charge car...
Nickel-based catalysts are promising for dry reforming of methane (DRM) owing to their high C─H bond activation ability and low cost, while highly susceptible to coke deposition and sintering. Here, we report a heteroenergetic Ce0.75Ti0.25O2-x support that simultaneously regulates Ni nanoparticle stabilization, DRM act...
Aliovalent A- and B-site co-doping of the Ruddlesden–Popper layered perovskite La2NiO4 is demonstrated as a rational strategy to tune redox properties and enhance catalytic performance in dry reforming of methane. Sr2+ substitution at the A-site of La1.6Sr0.4Ni1−yCuyO4 induces Ni2+ → Ni3+ oxidation and changes in the o...
Aathira Bhaskaran, Chandan Kumar Mandal, A. Gayen et al.· RSC Advances· 0 citations
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