Highly reactive and selective Sn-Pd bimetallic catalyst supported by nanocrystalline ZSM-5 for aqueous nitrate reduction

[Display omitted] •Nanocrystalline ZSM-5 supported bimetallic catalyst was developed to reduce NO3−.•Sn-Pd-NZSM-5 showed complete NO3− removal and high N2 selectivity in 1h.•Fast reduction kinetics was due to subsequent electron transfer from Sn0 and Sn2+.•Complete NO3− removal and high N2 selectivi...

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Veröffentlicht in:Applied catalysis. B, Environmental Environmental, 2016-06, Vol.187, p.37-46
Hauptverfasser: Hamid, Shanawar, Kumar, Macharla Arun, Lee, Woojin
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Kumar, Macharla Arun
Lee, Woojin
description [Display omitted] •Nanocrystalline ZSM-5 supported bimetallic catalyst was developed to reduce NO3−.•Sn-Pd-NZSM-5 showed complete NO3− removal and high N2 selectivity in 1h.•Fast reduction kinetics was due to subsequent electron transfer from Sn0 and Sn2+.•Complete NO3− removal and high N2 selectivity continued over five cycles. A new bimetallic catalyst supported by environmentally benign nanocrystalline ZSM-5 (NZSM-5), was developed to reduce nitrate completely and selectively to nitrogen gas without producing nitrite. The catalyst was optimized by use under a variety of conditions (i.e., promoter metal type (Sn, Cu, Ag, Ni)), noble metal type (Pd, Pt, Au), promoter metal concentration (0–3.4wt%), noble metal concentration (0–2.8wt%), catalyst calcination temperature (0–550°C), H2 flow rate (0–60mL/min), and CO2 flow rate (0–60mL/min). Complete nitrate removal with the highest nitrogen selectivity (91%) was achieved using 1%Sn-1.6%Pd-NZSM-5 catalyst under optimized conditions that included: initial nitrate concentration: 30mg/L NO3-N; calcination temperature: 350°C; H2 flow rate: 30mL/min; and CO2 flow rate: 60mL/min for 60min. The estimated kinetic rate constant of the catalyst is 16.40×10−2min−1, the catalyst-loading normalized rate constant is 65.60×10−2min−1gcat−1, while Pd-loading normalized rate constant is 410×10−2L/mingPd−1. The catalyst showed remarkable nitrate removal (100%) and nitrogen selectivity (>88%) for up to five successive reactions with consistent kinetics. A 100% nitrate removal and >81% nitrogen selectivity was also achieved by the catalyst for five repeated cycles. However, the kinetics gradually slowed down to 4.36×10−2min−1 over five repeated cycles, (still superior to fresh catalysts already reported in the literature). Characterization tests confirmed that the used catalyst was chemically stable, and that the decrease in its reactivity was due mainly to the sintering of metallic nano particles during the regeneration process.
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A new bimetallic catalyst supported by environmentally benign nanocrystalline ZSM-5 (NZSM-5), was developed to reduce nitrate completely and selectively to nitrogen gas without producing nitrite. The catalyst was optimized by use under a variety of conditions (i.e., promoter metal type (Sn, Cu, Ag, Ni)), noble metal type (Pd, Pt, Au), promoter metal concentration (0–3.4wt%), noble metal concentration (0–2.8wt%), catalyst calcination temperature (0–550°C), H2 flow rate (0–60mL/min), and CO2 flow rate (0–60mL/min). Complete nitrate removal with the highest nitrogen selectivity (91%) was achieved using 1%Sn-1.6%Pd-NZSM-5 catalyst under optimized conditions that included: initial nitrate concentration: 30mg/L NO3-N; calcination temperature: 350°C; H2 flow rate: 30mL/min; and CO2 flow rate: 60mL/min for 60min. The estimated kinetic rate constant of the catalyst is 16.40×10−2min−1, the catalyst-loading normalized rate constant is 65.60×10−2min−1gcat−1, while Pd-loading normalized rate constant is 410×10−2L/mingPd−1. The catalyst showed remarkable nitrate removal (100%) and nitrogen selectivity (&gt;88%) for up to five successive reactions with consistent kinetics. A 100% nitrate removal and &gt;81% nitrogen selectivity was also achieved by the catalyst for five repeated cycles. However, the kinetics gradually slowed down to 4.36×10−2min−1 over five repeated cycles, (still superior to fresh catalysts already reported in the literature). 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B, Environmental</title><description>[Display omitted] •Nanocrystalline ZSM-5 supported bimetallic catalyst was developed to reduce NO3−.•Sn-Pd-NZSM-5 showed complete NO3− removal and high N2 selectivity in 1h.•Fast reduction kinetics was due to subsequent electron transfer from Sn0 and Sn2+.•Complete NO3− removal and high N2 selectivity continued over five cycles. A new bimetallic catalyst supported by environmentally benign nanocrystalline ZSM-5 (NZSM-5), was developed to reduce nitrate completely and selectively to nitrogen gas without producing nitrite. The catalyst was optimized by use under a variety of conditions (i.e., promoter metal type (Sn, Cu, Ag, Ni)), noble metal type (Pd, Pt, Au), promoter metal concentration (0–3.4wt%), noble metal concentration (0–2.8wt%), catalyst calcination temperature (0–550°C), H2 flow rate (0–60mL/min), and CO2 flow rate (0–60mL/min). Complete nitrate removal with the highest nitrogen selectivity (91%) was achieved using 1%Sn-1.6%Pd-NZSM-5 catalyst under optimized conditions that included: initial nitrate concentration: 30mg/L NO3-N; calcination temperature: 350°C; H2 flow rate: 30mL/min; and CO2 flow rate: 60mL/min for 60min. The estimated kinetic rate constant of the catalyst is 16.40×10−2min−1, the catalyst-loading normalized rate constant is 65.60×10−2min−1gcat−1, while Pd-loading normalized rate constant is 410×10−2L/mingPd−1. The catalyst showed remarkable nitrate removal (100%) and nitrogen selectivity (&gt;88%) for up to five successive reactions with consistent kinetics. A 100% nitrate removal and &gt;81% nitrogen selectivity was also achieved by the catalyst for five repeated cycles. However, the kinetics gradually slowed down to 4.36×10−2min−1 over five repeated cycles, (still superior to fresh catalysts already reported in the literature). Characterization tests confirmed that the used catalyst was chemically stable, and that the decrease in its reactivity was due mainly to the sintering of metallic nano particles during the regeneration process.</description><subject>Catalysts</subject><subject>Catalytic nitrate reduction</subject><subject>Flow rate</subject><subject>Nanocrystalline ZSM-5 support</subject><subject>Nitrate removal</subject><subject>Nitrates</subject><subject>Nitrogen</subject><subject>Rate constants</subject><subject>Reaction kinetics</subject><subject>Selectivity</subject><subject>Sn-Pd bimetallic catalyst</subject><issn>0926-3373</issn><issn>1873-3883</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2016</creationdate><recordtype>article</recordtype><recordid>eNqFUU1v2zAMFYoOaJbtH-ygYy929W31UmAotqZAixbodtlFkGVqU-DInqQEy7-vAve8ngiSj--RfAh9oaSlhKqrbWtnZ0vfspq1hLaEyzO0orrjDdean6MVuWaq4bzjF-hjzltCCONMr9C_Tfj9ZzziBNaVcABs44AzjLBkL7F5HnAfdlDsOAaHq4wdj7ngvJ_nKRWo3SOONk4u1fIJFAH_enlsJPZTwvbvHqZ9xjGUZAtUnWFfqaf4CX3wdszw-S2u0c_v337cbpqHp7v7268PjROdLE1HGPNcKEavreJOaMVs7zy1PdPeDUwJ4SWvjV4R6XvGFSgrnJRcS6964Gt0ufDOaaq75GJ2ITsYRxtPixmqmRSaq_qm96FEq05roSpULFCXppwTeDOnsLPpaCgxJ0_M1iyemJMnhlBTPaljN8sY1IsPAZLJLkB0MIRUP26GKfyf4BXfHphN</recordid><startdate>20160615</startdate><enddate>20160615</enddate><creator>Hamid, Shanawar</creator><creator>Kumar, Macharla Arun</creator><creator>Lee, Woojin</creator><general>Elsevier B.V</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7ST</scope><scope>C1K</scope><scope>SOI</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>FR3</scope><scope>JG9</scope><scope>KR7</scope><scope>L7M</scope></search><sort><creationdate>20160615</creationdate><title>Highly reactive and selective Sn-Pd bimetallic catalyst supported by nanocrystalline ZSM-5 for aqueous nitrate reduction</title><author>Hamid, Shanawar ; Kumar, Macharla Arun ; Lee, Woojin</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c475t-7022f346219a63c4862abcf1ab28fcd2644f533c4b605fb236e6a4c55385f6be3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2016</creationdate><topic>Catalysts</topic><topic>Catalytic nitrate reduction</topic><topic>Flow rate</topic><topic>Nanocrystalline ZSM-5 support</topic><topic>Nitrate removal</topic><topic>Nitrates</topic><topic>Nitrogen</topic><topic>Rate constants</topic><topic>Reaction kinetics</topic><topic>Selectivity</topic><topic>Sn-Pd bimetallic catalyst</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Hamid, Shanawar</creatorcontrib><creatorcontrib>Kumar, Macharla Arun</creatorcontrib><creatorcontrib>Lee, Woojin</creatorcontrib><collection>CrossRef</collection><collection>Environment Abstracts</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Environment Abstracts</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Engineering Research Database</collection><collection>Materials Research Database</collection><collection>Civil Engineering Abstracts</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>Applied catalysis. B, Environmental</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Hamid, Shanawar</au><au>Kumar, Macharla Arun</au><au>Lee, Woojin</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Highly reactive and selective Sn-Pd bimetallic catalyst supported by nanocrystalline ZSM-5 for aqueous nitrate reduction</atitle><jtitle>Applied catalysis. B, Environmental</jtitle><date>2016-06-15</date><risdate>2016</risdate><volume>187</volume><spage>37</spage><epage>46</epage><pages>37-46</pages><issn>0926-3373</issn><eissn>1873-3883</eissn><abstract>[Display omitted] •Nanocrystalline ZSM-5 supported bimetallic catalyst was developed to reduce NO3−.•Sn-Pd-NZSM-5 showed complete NO3− removal and high N2 selectivity in 1h.•Fast reduction kinetics was due to subsequent electron transfer from Sn0 and Sn2+.•Complete NO3− removal and high N2 selectivity continued over five cycles. A new bimetallic catalyst supported by environmentally benign nanocrystalline ZSM-5 (NZSM-5), was developed to reduce nitrate completely and selectively to nitrogen gas without producing nitrite. The catalyst was optimized by use under a variety of conditions (i.e., promoter metal type (Sn, Cu, Ag, Ni)), noble metal type (Pd, Pt, Au), promoter metal concentration (0–3.4wt%), noble metal concentration (0–2.8wt%), catalyst calcination temperature (0–550°C), H2 flow rate (0–60mL/min), and CO2 flow rate (0–60mL/min). Complete nitrate removal with the highest nitrogen selectivity (91%) was achieved using 1%Sn-1.6%Pd-NZSM-5 catalyst under optimized conditions that included: initial nitrate concentration: 30mg/L NO3-N; calcination temperature: 350°C; H2 flow rate: 30mL/min; and CO2 flow rate: 60mL/min for 60min. The estimated kinetic rate constant of the catalyst is 16.40×10−2min−1, the catalyst-loading normalized rate constant is 65.60×10−2min−1gcat−1, while Pd-loading normalized rate constant is 410×10−2L/mingPd−1. The catalyst showed remarkable nitrate removal (100%) and nitrogen selectivity (&gt;88%) for up to five successive reactions with consistent kinetics. A 100% nitrate removal and &gt;81% nitrogen selectivity was also achieved by the catalyst for five repeated cycles. However, the kinetics gradually slowed down to 4.36×10−2min−1 over five repeated cycles, (still superior to fresh catalysts already reported in the literature). Characterization tests confirmed that the used catalyst was chemically stable, and that the decrease in its reactivity was due mainly to the sintering of metallic nano particles during the regeneration process.</abstract><pub>Elsevier B.V</pub><doi>10.1016/j.apcatb.2016.01.035</doi><tpages>10</tpages></addata></record>
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subjects Catalysts
Catalytic nitrate reduction
Flow rate
Nanocrystalline ZSM-5 support
Nitrate removal
Nitrates
Nitrogen
Rate constants
Reaction kinetics
Selectivity
Sn-Pd bimetallic catalyst
title Highly reactive and selective Sn-Pd bimetallic catalyst supported by nanocrystalline ZSM-5 for aqueous nitrate reduction
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