3D-Printed Boron Nitride Catalytic Monoliths for Oxidative Dehydrogenation of Propane

Agbi, Theodore O.; Lo, Wei-Shang; Baamran, Khaled; Ryu, Taekyung; Cheung, Christine; Rezaei, Fateme; Hermans, Ive

doi:10.1007/s11244-023-01819-2

Cited by 5 publications

(11 citation statements)

References 32 publications

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“…Intriguingly, supra-second-order alkane kinetics was also observed boron-based catalysts, such as 3D-printed hexagonal boron nitride monoliths, borosilicate zeolites, supported boron oxides, and boron phosphide, at certain operating conditions. The highest reported alkane reaction order is around 3 on boron oxide supported on SBA-15 with high boron loading (20 wt %) and boron phosphide. , According to eq , the occurrence of supra-second-order dependence with respect to the partial pressure of alkane means that the concentration of some important H-abstractors in the catalytic system has a second-order dependence on the partial pressure of the alkane.…”

Section: Deviations From the Second-order Kineticsmentioning

confidence: 88%

“…The first-order alkane kinetics was observed on B 2 O 3 /SBA-15 at low boron loading (<5 wt %) and low partial pressure of propane (<15 kPa), which is likely caused by the low radical concentration at such conditions. 63 Intriguingly, supra-second-order alkane kinetics was also observed boron-based catalysts, such as 3D-printed hexagonal boron nitride monoliths, 68 borosilicate zeolites, 67 supported boron oxides, 63 and boron phosphide, 33 at certain operating conditions. The highest reported alkane reaction order is around 3 on boron oxide supported on SBA-15 with high boron loading (20 wt %) and boron phosphide.…”

Section: Deviations From the Second-order Kineticsmentioning

confidence: 90%

“…The apparent activation energy of B-MFI and B-BEA is about 100 kJ·mol –1 , which is significantly lower than most bulk boron-based catalysts . Moreover, alkane reaction orders greater than two were reported on B 2 O 3 loaded on porous supports in recent studies. ,, Given the significant contribution from gas phase radicals to the ODH activity, common experimental strategies in heterogeneous catalysis such as titration of catalytic sites and identification of surface bound reaction intermediates are unlikely to be informative. Meanwhile, the unique and rich kinetic behavior of boron-catalyzed ODH could hold the key to gaining a mechanistic understanding.…”

Section: Shared Features Of Boron-based Odh Catalystsmentioning

confidence: 99%

“…When the dominant reaction pathway is shifted from surface-mediated mechanism to radical-mediated mechanism, the ODH activity per boron site is promoted and both Δ H ‡ and Δ S ‡ are increased. Considering the positive correlation between apparent activation energy and apparent alkane reaction order, this is also in line with the results that higher alkane reaction order corresponds to higher catalytic activity, as discussed in Section . ,,, …”

Section: Understanding Of the Apparent Activation Energymentioning

confidence: 99%

“…Existing studies suggest a general positive correlation between the alkane reaction order and the ODH activity, which could be attributed to the higher rates enabled by the gas-phase radical mechanism. 33,63,67,68…”

Section: Deviations From the Second-order Kineticsmentioning

confidence: 99%

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Kinetic Insights into Boron-Based Materials Catalyzed Oxidative Dehydrogenation of Light Alkanes

Tian,

2024

Precision Chemistry

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High selectivity toward alkenes in oxidative dehydrogenation (ODH) of light alkanes makes boron-based materials promising catalysts. However, many key mechanistic aspects are still debated due to the challenge of capturing fleeting reaction intermediates. Kinetic analysis, including determining reaction orders and activation energy, could be informative for reactions involving radical intermediates but has not been extensively exploited. This Review summarizes the current understanding of the apparent alkane reaction order and the apparent activation energy in the boron-catalyzed ODH. Despite varying compositions and structures, a majority of boron-based catalysts share many common features, including alkene selectivity, the evolution and the formation of active site, and the apparent kinetic properties. These common trends could be attributed to the shared gas-phase radical-mediated reaction pathways and the formation of active hydroxylated boron oxide species on boron-containing materials under ODH conditions. Values of apparent alkane reaction orders and apparent activation energies are sensitive and reliable experimental measures of the contributions of the gas-phase radicalmediated and surface-mediated pathways, suggesting the outline of a general mechanistic framework of the boron-catalyzed ODH.

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Section: Deviations From the Second-order Kineticsmentioning

confidence: 88%

Section: Deviations From the Second-order Kineticsmentioning

confidence: 90%

Section: Shared Features Of Boron-based Odh Catalystsmentioning

confidence: 99%

Section: Understanding Of the Apparent Activation Energymentioning

confidence: 99%

Section: Deviations From the Second-order Kineticsmentioning

confidence: 99%

See 3 more Smart Citations

Kinetic Insights into Boron-Based Materials Catalyzed Oxidative Dehydrogenation of Light Alkanes

Tian,

2024

Precision Chemistry

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Boosting gas-phase radical reactions for efficient oxidative dehydrogenation of propane over boron-based macropore catalyst

Qian,

Zhang,

Xiao

et al. 2024

Chemical Engineering Journal

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Reactive Carbon Capture: Cooperative and Bifunctional Adsorbent-Catalyst Materials and Process Integration for a New Carbon Economy

Baamran,

Lawson,

Rezaei

et al. 2024

Acc. Chem. Res.

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Metrics & MoreArticle Recommendations * sı Supporting Information CONSPECTUS: To say the least, releasing CO 2 into the atmosphere is reaping undue environmental consequences given the ever-present increase in severe global weather events over the past five years. However, it can be argued that−at least in the confines of current technological capabilities−the atmospheric release of CO 2 is somewhat unavoidable given that even shifting toward clean energy sources−such as solar, nuclear, wind, battery, or H 2 power−incurs an initial carbon requirement by way of manufacturing the very production abilities through which "clean" energy is generated. Even years from now, experts agree that energy production will be diversified and− as the global population continues to drive the growth of global energy consumption−thermal power derived from carbon combustion is likely to remain one intrinsic energetic source, of which CO 2 will always be a byproduct. In this context, it is the responsibility of the scientific community to devise improved pathways of carbon management such that (i) the consequences of combustion on the global environment are reduced and (ii) carbon fuels can be leveraged in a sustainable fashion.In this Account, we discuss a pivotal perspective shift on CO 2 emissions derived from a considerable breakthrough in material science from our work at Missouri University of Science and Technology. This account details the development of materials which no longer vilify CO 2 emissions as a valueless combustion byproduct, instead providing a path for them to become a potential feedstock. In more specific terms, this work details the development of structured, cooperative "bifunctional" materials (BFMs) comprised of (i) a high-temperature adsorbent and (ii) a heterogeneous catalyst that enable single-bed CO 2 capture and utilization in oxidative ethane dehydrogenation (ODHE), oxidative propane dehydrogenation (ODHP), and dry methane reforming (DMR) processes. This Account begins with the conceptual development of the BFMs in the powdered state, followed by detailing the firstever reports of structuring the materials into facile honeycomb contactors by 3D printing. The Account then summarizes the impressive performance of the 3D-printed BFMs, specifically focusing on how their catalysts (metal oxides and perovskites) influence their reactive CO 2 capture performances in ODHE, ODHP, and DMR processes. Such promise of CO 2 -as-fuel offers a glimpse into the future of a diversified energy economy, in which CO 2 /fuel looping can play an important role. A major factor in achieving this future is, of course, developing an appropriately active catalyst; an account of whose first breakthroughs in material science are detailed herein.

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3D-Printed Boron Nitride Catalytic Monoliths for Oxidative Dehydrogenation of Propane

Cited by 5 publications

References 32 publications

Kinetic Insights into Boron-Based Materials Catalyzed Oxidative Dehydrogenation of Light Alkanes

Kinetic Insights into Boron-Based Materials Catalyzed Oxidative Dehydrogenation of Light Alkanes

Boosting gas-phase radical reactions for efficient oxidative dehydrogenation of propane over boron-based macropore catalyst

Reactive Carbon Capture: Cooperative and Bifunctional Adsorbent-Catalyst Materials and Process Integration for a New Carbon Economy

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