[보고서]차세대 고연비 자동차 배기가스 정화용 촉매 시스템 개발

차세대 고연비 자동차 배기가스 정화용 촉매 시스템 개발
Emission Control Catalytic System for Next Generation Energy-Efficient Vehicle 원문보기

보고서 정보
주관연구기관	포항공과대학교 Pohang University of Science and Technology
보고서유형	최종보고서
발행국가	대한민국
언어	한국어
발행년월	2014-09
과제시작연도	2013
주관부처	미래창조과학부 Ministry of Science, ICT and Future Planning
등록번호	TRKO201400028592
과제고유번호	1711001149
사업명	중견연구자지원
DB 구축일자	2014-11-22
키워드	환경촉매.기솔린/디젤.고효율/고연비 차세대 엔진.배기가스 규제.선택적 촉매 환원법.NO 산화 촉매.삼원촉매.반응 속도론 및 반응기 모델.Lean NOx Trap.Environmental catalyst.Gasoline/Diesel.Fuel-efficient vehicle.Emission regulation.Urea or HC/SCR.NO oxidation catalyst.Three-way catalyst.Reaction kinetics.
DOI	https://doi.org/10.23000/TRKO201400028592

초록 ▼

제1과제에서는 Urea/SCR 촉매 시스템의 차세대 엔진 적용을 위하여 새로운 종류의 Mn 기반 저온 촉매의 개발에 성공하였으며, 최근 개발되어 가장 유망한 저온 SCR 촉매로 각광을 받고 있는 small pore zeolite 기반 촉매의 우수한 열적내구성의 원인을 규명하고, 최종적으로 상기 촉매의 deNOx 활성을 모사할 수 있는 kinetic model을 개발하였다. 제2과제에서는 HC/SCR 기술의 상용화에 대한 가장 큰 문제점인 낮은 저온 활성을 반응가스 내 OHC/H₂의 주입, monoethanolamine의 환원제 적용 및 지지체의 개선에 의한 촉매 산점증진으로 향상시켰으며 최종적으로 HC/SCR의 활성을 예측할 수 있는 kinetic model을 개발하여 reaction mechanism의 규명 및 향후 HC/SCR 기술의 상용화를 위한 기틀을 마련하였다. 제3과제에서 는 LNT 기술의 단점인 취약한 촉매 SO₂ 내구성을 극복하고자 Li-Al 기반의 촉매를 개발하였으며, 높은 촉매 개발단가를 절감하기 위하여 high-throughput combichem 방법을 적용하여 고가의 Pt를 대체할 수 있는 perovskite 기반의 NO 산화 촉매를 개발하고 LNT 적용 가능성을 열어 놓았다. 제4과제에서는 가솔린 배기가스 정화를 위해 사용되고 있는 상용 TWC 의 성능을 noble metal 함량 및 촉매 mileage에 따라 종합적으로 모사할 수 있는 kinetic model 및 activity function을 개발하여 실제 자동차 촉매 converter 설계를 위한 유용한 tool 로서 가이드라인을 제시하고자 하였으며, 추가적으로 촉매의 열적 내구성 개선을 통하여 주금속으로 사용되는 값비싼 noble metal의 사용량을 절감하고자 하였다. 제5과제에서는 각 세부과제의 목표달성을 위하여 필요한 촉매들을 nanochemistry 기법에 기반하여 제조하였고, 이를 통한 자체 촉매 제조 기술 자립화를 위한 연구를 진행하였다.

Abstract ▼

For the application of Urea/SCR technology to the next-generation fuel-efficient automotive engine, a new generation of Mn-based low temperature SCR catalyst has been developed. In addition, the cause behind the exceptionally strong hydrothermal stability of CuSSZ13 catalyst, currently drawing keen interest from the auto industry, has been elucidated, and the reaction kinetics for describing its deNOx activity has been also developed. In order to enhance the low-temperature HC/SCR activity, the improvement of the deNOx performance upon the addition of OHC/H₂ into feed gas stream, the use of bifunctional reductant as well as the modification of catalyst support have been investigated. Furthermore, the kinetic study for developing the reaction kinetics for HC/SCR reaction has been also conducted. For the LNT technology, the sulfur tolerant Li-Al based catalyst has been developed.
In addition, the perovskite based NO oxidation catalyst to replace the high cost Pt-based counterpart has been developed by the high-throughput combichem method and its feasibility to be applied to the LNT system has been also determined. The 3D activity functions for the commercial Pd-based TWC have been successfully developed to predict the TWC performance with respect to the Pd contents and catalyst mileages. Furthermore, the thermal stable Rh/ZrO₂ and LaAlPdO₃ catalysts have been developed as an alternative TWC. All catalysts employed in this study have been prepared on the basis of the concept of nanotechnology.

표/그림 (72)

표 Emission standards for gasoline vehicles [2].
표 Emission standards for heavy-duty diesel vehicles [3].
표 XRD patterns of TiO2 and Mn/TiO2 catalyst.
표 DeNOx activity (a) and N2 selectivity (b) over the Mn-based and CuZSM5 catalysts. Feed gas composition: 500 ppm NO, 500 ppm NH3, 5% O2, 10% H2O and N2 balance. GHSV=100,000 h-1. N2 selectivity=[(conversion of NO+NH3)-(formation of N2O+NO2)]/(conversion of NO+NH3).
표 XPS of Mn 2p core level (a) and NH3-TPD (b) over the Mn-based catalysts.
표 Mn 2p XPS spectra of the Mn-based ZSM5 catalysts before/after aging.
표 Mn/SM rCaatitoa of the catalysts obtained from XPS peak area of each component
표 ESR spectra of CuSSZ-13 catalyst before and after aging.
표 Effect of Cu content (a) and Si/Al ratio (b) on the hydrothermal stability of CuSSZ13 catalyst. Feed gas composition: 500 ppm NO, 500 ppm NH3, 5% O2, 10% H2O, and N2 balance. GHSV=100,000 h-1. Aging condition: at 850 oC for 24h with flowing air containing 10% H2O.
표 Deconvolution of ESR spectra over CuSSZ 13 before (a) and after (b) aging at 850 oC.
표 Distribution of Cu2+ species on the catalysts determined by ESR analysis
표 Cu K-edge XANES spectra for the CuSSZ13 catalysts before (a) and after (b) aging at 850oC.
표 Reduction of nitrate species by NO on CuSSZ13 catalyst (DRIFT study). Pre-adsorption: 500 ppm NO2 in Ar balance at 200oC for 1h. Feed gas composition: 500 ppm NO in Ar balance. Temperature: 200 oC.
표 Consumption of NH3 adsorbed onto CuSSZ13 catalyst by NO (a) and NO2 (b) (DRIFT study). Pre-adsorption: 500 ppm NH3 in Ar balance at 200 oC for 1 h. Feed gas composition: 500 ppm NO (a) or 500 ppm NO2 (b) in Ar balance. Temperature: 200 oC.
표 Reactant adsorption and desorption over CuSSZ13 catalyst
표 Surface reaction mechanism over CuSSZ13 catalyst
표 UV-vis spectra over Ag/Al2O3 catalysts with respect to the Ag loading.
표 Ratio of ionic Ag and metallic Ag for Ag/Al2O3 catalysts
표 H2 TPR profiles of Ag/Al2O3 catalysts with respect to Ag loading.
표 Amount of H2 consumption per Ag included in Ag/Al2O3 catalysts by TPR
표 Comparison of UV-vis spectra of the Ag(3.8)/Al2O3 catalyst with or without H2 in the feed at 200 ℃
표 Comparison of NOx conversion by various reductants over the Ag(3.8)/Al2O3 catalyst. Feed gas composition: 400 ppm NO, 400 ppm NH2(CH2)2OH or 400 ppm C2H5OH + 400 ppm NH3 or 400ppm C2H5OH or 400 ppm NH3, 6% O2, 2.5% H2O and He balance. GHSV=60,000 h-1.
표 Comparison of UV-vis spectra over Ag(3.8)/Al2O3 and Ag(3.8)/AlF3(F:2.7)/Al2O3 catalysts.
표 HOCH2CH2NH2 oxidation over Ag(3.8)/Al2O3 catalyst. Feed gas composition: 400 ppm HOCH2CH2NH2, 6% O2, 2.5% H2O, and He balance. Catalyst: 20/30 mesh, 1 g. GHSV=60,000 h-1.
표 Reactant adsorption and desorption over Ag(3.8)/Al2O3 catalyst
표 Ethanol oxidation activity over Ag(3.8)/Al2O3, Ag(~4.0)/W(~6.0)/Al2O3; ethanol conversion
표 H2 TPR profiles of Li-Al- and Al2O3-based catalysts.
표 FT-IR spectra of Al2O3-based catalyst under oxidizing wet/dry and wet conditions.
표 FT-IR spectra of Li-Al-based catalyst under oxidizing wet/dry and wet conditions.
표 The amount of H2O adsorbed onto Li-Al and Al2O3 supports
표 NOx conversion over Li-Al-and Al2O3-based LNT monoliths. Lean condition (50s): 8% O2, 330 ppm NO, 10% H2O, 5% CO2, Ar balance, rich condition (10s): 1% O2, 330 ppm NO, 0.2% CO, 4000 ppm C3H6, 10% H2O, 5% CO2, Ar balance. GHSV= 60,000h-1.
표 Summary of NO oxidation performances and amount of NO2 produced by perovskites
표 Correlation between NO-to-NO2 conversion and the amount of NO2 produced by perovskite catalysts.
표 The amount of NOx trapped onto the K/Al2O3 by the NO oxidation over the perovskite catalysts at 200 oC.
표 Effect of CO and C3H6 on NO oxidation activity
표 Comparison of the price for the catalyst preparations
표 NO oxidation activity over degreened single- and dual-bed reactor system. Feed gas composition: 400 ppm NO, 8% O2, 10% H2O, 1,000 ppm CO, 1,000 ppm C1 C3H6 (333 ppm) and N2 balance. GHSV=60,000 h-1.
표 TWC activities over 4k, 41k and 98k Pd140 catalysts. Feed gas composition: 1% CO, 500 ppm C3H6, 0.3% H2, 1% O2, 500 ppm NO, 10% CO2, 10% H2O and Ar balance (S=1.17). GHSV=100,000 h-1.
표 XRD patterns over fresh and aged TWCs; (a) Pd200 and (b) Pd280 TWCs.
표 Alteration of physical properties of Pd TWCs
표 Alteration of Pd MSA as a function of the catalyst mileage over the Pd80 catalyst
표 Model prediction of catalytic activity by using the activity function.
표 Dispersion and MSA of Pd over the 4k Pd TWCs as a function of Pd loading
표 Effect of Pd loading on the TWC performance over the 4k Pd20, 80, 160 and 240 (g/ft3). Feed gas composition: 1% CO, 0.3% H2, 500 ppm C3H6, 1% O2, 500 ppm NO, 10% CO2, 10% H2O and Ar balance (S=1.17). GHSV=100,000 h-1.
표 Model prediction of catalytic activity by using activity function.
표 The prediction of TWC performance over the 4k Pd TWC with respect to the Pd loading. Feed gas composition: 1% CO, 0.3% H2, 500 ppm C3H6, 1% O2, 500 ppm NO, 10% CO2, 10% H2O and Ar balance (S=1.17). GHSV=100,000 h-1.
표 Physicochemical properties of Rh/ZrO2 catalysts
표 XRD patterns over fresh and aged Rh/ZrO2 catalysts; (○) monoclinic and (■) tetragonal phase.
표 XPS spectra (Rh 3d) (a) and H2-TPR profiles (b) over fresh and aged Rh/ZrO2 catalysts.
표 Effect of reducing pretreatment on the alteration of the Rh MSA over the Rh-based catalyst.
표 T50 (CO, C3H6, H2) and T20 (NO) over 4k and aged Pd catalysts. Feed gas composition: 1% CO, 0.3% H2, 500 ppm C3H6, 500 ppm NO, 1% O2, 10% CO2, 10% H2O, and Ar balance (S=1.17). GHSV=100,000 h-1.
표 Physicochemical properties of Pd catalysts
표 TG profiles over Pd catalysts.
표 Sub-ambient H2-TPR profiles of Pd catalysts.
표 H2 consumption over Pd catalysts.
표 TWC performance of commercial Pdc1 catalysts as a function of both Pd loading and catalyst mileage. Feed gas composition: 1% CO, 500 ppm C3H6, 0.3% H2, 1% O2, 500 ppm NO, 10% CO2, 10% H2O and Ar balance (S=1.17). GHSV=100,000 h-1.
표 The prediction of TWC performance over the Pdc1 catalyst as a function of both Pd loading and catalyst mileage. Feed gas composition: 1% CO, 0.3% H2, 500 ppm C3H6, 1% O2, 500 ppm NO, 10% CO2, 10% H2O and Ar balance (S=1.17).
표 Pd 3d XPS spectra of Pd catalysts.
표 Pd 3d5/2 binding energy and surface atomic ratio of Pd catalysts
표 DRIFT spectra over Pd catalysts. Feed gas composition: 1% CO and He balance for 30 min at 35 oC.
표 Zeta potential of C1Z3 and Al2O3 as function of pH of precursor solution.
표 Light-off curves for CO, C3H6, O2 and NO conversion, and N2O and NH3 formation over fresh (closed symbol) and aged (open symbol) Pd catalysts. Feed gas composition: 1% CO, 0.3% H2, 500 ppm C3H6, 500 ppm NO, 1% O2, 10% CO2, 10% H2O, and Ar balance. GHSV= 100,000 h-1.
표 CO chemisorption results of fresh and aging Pd catalysts
표 TGA/DTA traces of as-made (a) K+ and (b) Na+- exchanged forms of GaNAT.
표 Dual-cycle, bimolecular and monomolecular ethyl-transfer reaction mechanism for zeolite-catalyzed ethylbenzene disproportionation.
표 XRD patterns of SSZ13 synthesized w.r.t. Si/Al ratio.
표 27Si-MAS-NMR spectra of SSZ13 synthesized w.r.t. Si/Al ratio.
표 List of chemical employed in the catalyst synthesis
표 TPD profiles over as-prepared La0.9Sr0.1MnO3 catalyst.
표 XRD patterns of perovskite-based catalysts.
표 Configuration of LNT monoliths
표 Configuration of TWC monoliths.

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차세대 고연비 자동차 배기가스 정화용 촉매 시스템 개발
Emission Control Catalytic System for Next Generation Energy-Efficient Vehicle 원문보기

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차세대 고연비 자동차 배기가스 정화용 촉매 시스템 개발 Emission Control Catalytic System for Next Generation Energy-Efficient Vehicle 원문보기

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차세대 고연비 자동차 배기가스 정화용 촉매 시스템 개발
Emission Control Catalytic System for Next Generation Energy-Efficient Vehicle 원문보기

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