scholarly journals Correction to “CO2 Chemisorption and Its Effect on Methane Activation in La2O3-Catalyzed Oxidative Coupling of Methane”

2016 ◽  
Vol 120 (17) ◽  
pp. 9545-9545
Author(s):  
Changqing Chu ◽  
Yonghui Zhao ◽  
Shenggang Li ◽  
Yuhan Sun
2021 ◽  
Vol 118 (23) ◽  
pp. e2012666118
Author(s):  
Shanfu Liu ◽  
Sagar Udyavara ◽  
Chi Zhang ◽  
Matthias Peter ◽  
Tracy L. Lohr ◽  
...  

The oxidative coupling of methane to ethylene using gaseous disulfur (2CH4 + S2 → C2H4 + 2H2S) as an oxidant (SOCM) proceeds with promising selectivity. Here, we report detailed experimental and theoretical studies that examine the mechanism for the conversion of CH4 to C2H4 over an Fe3O4-derived FeS2 catalyst achieving a promising ethylene selectivity of 33%. We compare and contrast these results with those for the highly exothermic oxidative coupling of methane (OCM) using O2 (2CH4 + O2 → C2H4 + 2H2O). SOCM kinetic/mechanistic analysis, along with density functional theory results, indicate that ethylene is produced as a primary product of methane activation, proceeding predominantly via CH2 coupling over dimeric S–S moieties that bridge Fe surface sites, and to a lesser degree, on heavily sulfided mononuclear sites. In contrast to and unlike OCM, the overoxidized CS2 by-product forms predominantly via CH4 oxidation, rather than from C2 products, through a series of C–H activation and S-addition steps at adsorbed sulfur sites on the FeS2 surface. The experimental rates for methane conversion are first order in both CH4 and S2, consistent with the involvement of two S sites in the rate-determining methane C–H activation step, with a CD4/CH4 kinetic isotope effect of 1.78. The experimental apparent activation energy for methane conversion is 66 ± 8 kJ/mol, significantly lower than for CH4 oxidative coupling with O2. The computed methane activation barrier, rate orders, and kinetic isotope values are consistent with experiment. All evidence indicates that SOCM proceeds via a very different pathway than that of OCM.


ACS Catalysis ◽  
2018 ◽  
Vol 8 (12) ◽  
pp. 11761-11772 ◽  
Author(s):  
Zebang Liu ◽  
Jerry Pui Ho Li ◽  
Evgeny Vovk ◽  
Yan Zhu ◽  
Shenggang Li ◽  
...  

2019 ◽  
Vol 9 (6) ◽  
pp. 1349-1356 ◽  
Author(s):  
Johnny Zhu Chen ◽  
Zhenwei Wu ◽  
Xiaoben Zhang ◽  
Slgi Choi ◽  
Yang Xiao ◽  
...  

Identification of a Pt3Bi nanoscale, surface intermetallic alloy catalyst for non-oxidative coupling of methane (NOCM).


2021 ◽  
Author(s):  
P. Saychu ◽  
M. Thanasiriruk ◽  
C. Khajonvittayakul ◽  
R. Viratikul ◽  
V. Tongnan ◽  
...  

Catalysts ◽  
2021 ◽  
Vol 11 (3) ◽  
pp. 388
Author(s):  
Yuqiao Fan ◽  
Changxi Miao ◽  
Yinghong Yue ◽  
Weiming Hua ◽  
Zi Gao

In this work, Ho2O3 nanosheets were synthesized by a hydrothermal method. A series of Sr-modified Ho2O3 nanosheets (Sr-Ho2O3-NS) with a Sr/Ho molar ratio between 0.02 and 0.06 were prepared via an impregnation method. These catalysts were characterized by several techniques such as XRD, N2 adsorption, SEM, TEM, XPS, O2-TPD (temperature-programmed desorption), and CO2-TPD, and they were studied with respect to their performances in the oxidative coupling of methane (OCM). In contrast to Ho2O3 nanoparticles, Ho2O3 nanosheets display greater CH4 conversion and C2-C3 selectivity, which could be related to the preferentially exposed (222) facet on the surface of the latter catalyst. The incorporation of small amounts of Sr into Ho2O3 nanosheets leads to a higher ratio of (O− + O2−)/O2− as well as an enhanced amount of chemisorbed oxygen species and moderate basic sites, which in turn improves the OCM performance. The optimal catalytic behavior is achievable on the 0.04Sr-Ho2O3-NS catalyst with a Sr/Ho molar ratio of 0.04, which gives a 24.0% conversion of CH4 with 56.7% selectivity to C2-C3 at 650 °C. The C2-C3 yield is well correlated with the amount of moderate basic sites present on the catalysts.


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