PdAu-catalyzed oxidation through in situ generated H2O2 in simulated produced water

Yin, Y. Ben; Heck, Kimberly N.; Coonrod, Christian L.; Powell, Camilah D.; Guo, Sujin; Reynolds, Michael A.; Wong, Michael S.

doi:10.1016/j.cattod.2019.05.001

Cited by 12 publications

(9 citation statements)

References 41 publications

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“…PdAu dropped 50% in activity, indicating its greater resistance to chloride interference. The improved salinity resistance may be attributed to weaker chloride chemisorption onto the bimetallic surface as reported elsewhere. , …”

Section: Resultssupporting

confidence: 69%

“…All three catalysts (i.e., PdAu/Al 2 O 3 , Pd/Al 2 O 3 , and Au/Al 2 O 3 ) were ground by mortar and pestle and sieved into fine powders with a particle size less than 300 μm (U.S. standard 50 mesh). The PdAu, Pd, and Au NPs had a uniform size distribution with mean diameters of 3.7 ± 0.3, 2.7 ± 0.4, and 3.4 ± 0.4 nm, respectively, as characterized by TEM in our previous work . TEM and XRD characterizations of catalysts are provided in Supporting Information (SI).…”

Section: Methodsmentioning

confidence: 93%

“…Recently, we found that a bimetallic PdAu catalyst has activity for the oxidative degradation of a model organic compound in simulated HFPW in the presence of formic acid (an organic contaminant found in HFPW) and air . We showed that the catalyst generated H 2 O 2 (and hydroxyl radicals, • OH) during the reaction as the oxidant over a wide range of salinities.…”

Section: Introductionmentioning

confidence: 97%

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Room-Temperature Catalytic Treatment of High-Salinity Produced Water at Neutral pH

Yin

Coonrod

Heck

et al. 2020

Ind. Eng. Chem. Res.

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Produced waters from hydraulic fracturing (HFPW) operations greatly challenge traditional water treatment technologies due to the high concentrations of total dissolved solids (TDS), highly complex and variable water matrices, and significant residual hydrocarbon content. We recently reported the unusual ability of a PdAu catalyst to degrade phenol in simulated HFPW at room temperature by generating H 2 O 2 in situ from formic acid and air. Phenol removal occurred at TDS levels as high as ∼10 000 ppm (ionic strength I = 0.3 M), but the catalytic reaction required pH < 4 to proceed. Here, we find that PdAu, Pd, and Au degraded phenol in the pH 5−8 range by using hydroxylamine as the hydrogen source in place of formic acid. Pd exhibited the highest activity, and Au the least. Activity of the monometallic catalysts decreased >70% as TDS increased from 0 to ∼100 000 ppm (I = 3 M), whereas the PdAu was comparatively less affected (∼50% activity decrease). All catalysts remained active at TDS levels as high as 100 000 ppm. The majority of the hydroxylamine formed N 2 , however this reaction generated additional nitrite/nitrate anion byproducts with nitrogen selectivities ranging from 0.5% to 11.5%, depending on the catalyst identity and reaction salinity. To demonstrate one possible flow treatment process concept, we constructed and tested a recirculating trickle bed reactor that removed 28% phenol from simulated HFPW over 48 h. These results show the potential of oxidation catalysis as a treatment approach for produced water and other high-salinity industrial wastewaters.

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Section: Resultssupporting

confidence: 69%

Section: Methodsmentioning

confidence: 93%

Section: Introductionmentioning

confidence: 97%

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Room-Temperature Catalytic Treatment of High-Salinity Produced Water at Neutral pH

Yin

Coonrod

Heck

et al. 2020

Ind. Eng. Chem. Res.

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“…Bimetallic catalysts often exhibit enhanced catalytic performance compared to their monometallic counterparts and are widely used in many chemical transformations including reforming 1 , 2 , coupling 3 , pollution control 4 , 5 , and oxidation 6 , 7 reactions. The specific reactivity of bimetallic catalysts is generally explained via ensemble (geometric) and/or ligand (electronic) effects that lead to enhanced reactivity and/or selectivity 8 – 10 .…”

Section: Introductionmentioning

confidence: 99%

Directing reaction pathways via in situ control of active site geometries in PdAu single-atom alloy catalysts

et al. 2021

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The atomic scale structure of the active sites in heterogeneous catalysts is central to their reactivity and selectivity. Therefore, understanding active site stability and evolution under different reaction conditions is key to the design of efficient and robust catalysts. Herein we describe theoretical calculations which predict that carbon monoxide can be used to stabilize different active site geometries in bimetallic alloys and then demonstrate experimentally that the same PdAu bimetallic catalyst can be transitioned between a single-atom alloy and a Pd cluster phase. Each state of the catalyst exhibits distinct selectivity for the dehydrogenation of ethanol reaction with the single-atom alloy phase exhibiting high selectivity to acetaldehyde and hydrogen versus a range of products from Pd clusters. First-principles based Monte Carlo calculations explain the origin of this active site ensemble size tuning effect, and this work serves as a demonstration of what should be a general phenomenon that enables in situ control over catalyst selectivity.

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“…In situ chemical generation and byproduct formation is not well understood in the context of resource extraction waters. 194…”

Section: Challengesmentioning

confidence: 99%

National Alliance for Water Innovation (NAWI) Resource Extraction Sector Technology Roadmap 2021

Cath

Chellam

Katz

et al. 2021

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Industrial WastewaterWater from various industrial processes that can be treated for reused Municipal WastewaterWastewater treated for reuse through municipal resource recovery treatment plants utilizing advanced treatment processes or decentralized treatment systems Agricultural WastewaterWastewater from tile drainage, tailwater, and other water produced on irrigated croplands as well as wastewater generated during livestock management that can be treated for reuse or disposal to the environment Mining WastewaterWastewater from mining operations that can be reused or prepared for disposal Produced WaterWater used for or produced by oil and gas exploration activities (including fracking) that can be reused or prepared for disposal Power and Cooling WastewaterWater used for cooling or as a byproduct of treatment (e.g., flue gas desulfurization) that can be reused or prepared for disposal PowerWater used in the electricity sector, especially for thermoelectric cooling Resource ExtractionWater used to extract resources, including mining and oil and gas exploration and production IndustrialWater used in industrial and manufacturing activities not included elsewhere, including but not limited to petrochemical refining, food and beverage processing, metallurgy, and commercial and institutional building cooling MunicipalWater used by public water systems, which include entities that are both publicly and privately owned, to supply customers in their service area

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PdAu-catalyzed oxidation through in situ generated H2O2 in simulated produced water

Cited by 12 publications

References 41 publications

Room-Temperature Catalytic Treatment of High-Salinity Produced Water at Neutral pH

Room-Temperature Catalytic Treatment of High-Salinity Produced Water at Neutral pH

Directing reaction pathways via in situ control of active site geometries in PdAu single-atom alloy catalysts

National Alliance for Water Innovation (NAWI) Resource Extraction Sector Technology Roadmap 2021

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