Synthesize and investigate the catalytic activity of three - Way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine

Figure 3.50 showed the activity of precious catalyst supported on Al2O3. The precious catalyst with the Pd loading content of 0.5% wt exhibited approximate 40% CO conversion at temperature from 150 to 350 oC. At higher temperature, this sample converted completely CO. C3H6, NO conversion of this catalyst reached maximum value (97% and 80%, respectively) from 350 oC. Meanwhile, 40% wt MnCoCe supported on γ-Al2O3 exhibited maximum conversion of CO, NO and C3H6 correspond 200, 250, and 300 oC. Thus, the use of noble metal Pd was not as effective as MnCeCo in this case due to the small precious metal loading on support. 0.5% wt Pd catalyst converted CO, C3H6 and NO at much higher temperature than that of the optimal 40% MnCoCe on Al2O3. The maximum pollutant conversions on both catalysts are approximately the same. Moreover, an equal activity to noble catalyst sample is already obtained for the MnCoCe sample containing only 20-30% active phase on the support.

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so able to treat completely soot within 7 hours on stream (4.35% CO, 7.06% O2, 1.15% C3H6, 1.77% NO). However, the presence of soot led to slightly decrease of activity after 5 hours on stream. It could be improved when the ratio of catalyst-soot is increased. In fact, a ratio of 10/1, which is suitable with a real application, results in only a little decrease of activity. 4. The study on different MnO2-Co3O4-CeO2 catalyst with altering MnO2/Co3O4/CeO2 composition revealed that only mixture with MnO2-Co3O4=1-3 exhibited the distinguished activity. Moreover, composition of CeO2 should be reasonable (CeO2/MnO2 from 0.38 to 1.26) to ensure the best activity. The addition of the fourth element in the catalyst resulted to decrease activity. MnO2-Co3O4-NiO catalysts were also studied and showed good activity but still less than that of MnO2-Co3O4-CeO2. 5. Effort to increase ability to treat NO by adding BaO and WO3 showed that NO conversion was improved slightly by adding 10% BaO but CO and hydrocarbon conversion decreased accordingly. 6. Investigation of MnO2-Co3O4-CeO2 activity after aging under H2O and SO2 at high temperature showed that the catalytic activity at low reaction temperature decreased significantly after aging but remained at high temperatures (>250 oC). The addition of ZrO2 did not prevent this decrease as expected. The catalyst MnO2-Co3O4-CeO2 1-3-0.75 not only remained its catalytic activity at high temperature above 500 oC but also converted CO and C3H6 at low temperature after activation in the flow with O2/CO=1.6 at 100 oC. The catalyst was able to treat 100% CO and approximate 100% C3H6 without CO2 in the gas flow from room temperature. Furthermore, the catalyst can convert 100% CO and 98.56% C3H6 with the presence of CO2 in the reaction flow. 7. 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Haneda, Nitin Labhsetwar (2008) Co3O4–CeO2 mixed oxide-based catalytic materials for diesel soot oxidation, Catalysis Today 132 (2008) 188–193 126 pollution 127 pollute.1.6529573.html Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 100 LIST OF PUBLISHMENTS 1 Nguyễn Thế Tiến, Nguyễn Thị Ái Nghĩa, Phạm Thị Mai Phương, Đỗ Văn Hưng, Isabel Van Driessche, Lê Minh Thắng (2012) Xúc tác trên cơ sở oxit kim loại xử lý muội trong khí thải động cơ đốt trong, Tạp chí Hóa học 50(4A), tr. 371-374 2 Nguyễn Thế Tiến, Nguyễn Thị Ái Nghĩa, Phạm Thị Mai Phương, Đỗ Văn Hưng, Nguyễn Duy Vinh, Isabel Van Driessche, Lê Minh Thắng (2012) Hoạt tính các hệ xúc tác trên cơ sở đơn oxit kim loại cho quá trình xử lý hydrocacbon trong khí thải xe máy, Tạp chí Hóa học 50(5B), tr.88-92 3 Nguyễn Thế Tiến, Phạm Thị Mai Phương, Lê Minh Thắng, Isabel Van Driessche (2013) Ảnh hưởng của BaO và WO3 đến hoạt tính của hệ xúc tác đa oxit kim loại xử lý khí thải động cơ đốt trong, Tạp chí Hóa học 51(2C), tr. 967-970 4 Tien Nguyen The, Phuong Pham Thi Mai, Thang Le Minh, Isabel Van Driessche (2013) Catalyst based on mixtures of CeO2-ZrO2 for propylene complete oxidation, Tạp chí xúc tác và hấp phụ 2(2), tr. 176-181 5 Tien The Nguyen, Phuong Thi Mai Pham, Thang Minh Le, Isabel Van Driessche (2013) Catalytic Activity of MnO2-Co3O4 for Complete Oxidation of Propylene, Kỷ yếu hội nghị quốc tế ICEM11- Đại học Bách Khoa Hà Nội, tr. 146-151 6 Nguyễn Thế Tiến, Nguyễn Xuân Dũng, Phạm Thị Mai Phương, Lê Minh Thắng, Isabel Van Driessche (2013) Ảnh hưởng của quá trình già hóa đến hệ xúc tác trên cơ sở oxit hỗn hợp MnO2-Co3O4-CeO2, Tạp chí Hóa học 51(6ABC), tr. 376-379 Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 101 ANNEX Annex 1 Complete oxidation of C3H6 and CO in deficient oxygen condition Annex 1.1 Complete oxidation of C3H6 in deficient oxygen condition 0 10 20 30 40 250 300 350 400 450 Reaction temperature, oC C 3H 6 c on ve rs io n, % Co3O4 MnCo 1-9 MnCo 1-4 MnCo 1-3 MnCo 1-1 MnCo 7-3 MnCo 9-1 MnO2 Figure A1: C3H6 conversion of MnCo samples in deficient oxygen condition (O2/C3H6=1/1) 0 20 40 60 80 100 250 300 350 400 450 Reaction temperature, oC C O 2 s el ec tiv ity , % Co3O4 MnCo 1-9 MnCo 1-4 MnCo 1-3 MnCo 1-1 MnCo 7-3 MnCo 9-1 MnO2 Figure A2: CO2 selectivity of MnCo samples in deficient oxygen condition (O2/C3H6=1/1) a b Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 102 c d Figure A3: SEM images of MnCo 1-3, MnCo 7-3 before (a,c) and after reaction (b,d) in deficient oxygen condition (O2/C3H6=1/1) 0 5 10 15 20 25 30 35 40 45 150 200 250 300 350 400 450 500 550 Temperature (oC) pr op yl en e co nv er si on (% ) Co3O4 10% CeO2 20% CeO2 50% CeO2 CeO2 Figure A4: C3H6 conversion of CeO2-Co3O4 chemical mixtures at different reaction temperatures in deficient oxygen condition (O2/C3H6=1/1) 30 40 50 60 70 80 90 100 150 200 250 300 350 400 450 500 550 Temperature (oC) CO 2 se le ct iv ity (% ) Co3O4 10% CeO2 20% CeO2 50% CeO2 CeO2 Figure A5 CO2 selectivity of CeO2-Co3O4 chemical mixtures depend on temperaturesin deficient oxygen condition (O2/C3H6=1/1) Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 103 0 20 40 60 80 100 1 1.5 2 3 4 5 6 O2/C3H8 ratio sufficient oxygen C 3H 8 c on ve rs io n, % 200 oC 250 oC 300 oC 350 oC 400 oC 450 oC 500 oC max conversion Figure A6: C3H8 conversion of MnCoCe 1-3-0.75 depends on O2/C3H8 ratio at different reaction temperatures (max conversion is the conversion correspond CO2 selectivity reach 100% in the reaction C3H8 + 5O2→ 3CO2 +4 H2O) Annex 1.2 Complete oxidation of CO in deficient oxygen condition Annex 1.2.1 Characterization and catalytic activity of single metallic oxides Table A1 Specific surface area of some single metallic oxides Samples CeO2 ZrO2 Co3O4 MnO2 NiO CuO SnO2 V2O5 ZnO SBET (m2/g) 33 52.34 11.39 5.61 10.81 2.17 16.66 3.89 13.62 50 40 30 20 10 In te ns ity , a .u 80706050403020 2theta, degrees MnO2 MnO2 MnO2 MnO2 MnO2 400 350 300 250 In te ns ity , a .u 706050403020 2theta, degrees Co3O4 Co3O4 Co3O4 Co3O4 Co3O4 a b Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 104 1400 1200 1000 800 600 400 200 0 In te ns ity , a .u 706050403020 2theta, degree NiO NiO NiO Ni2O3 100 80 60 40 20 In te ns ity , a .u 80706050403020 2 theta, degrees CuO CuO CuO CuO CuO c d 400 300 200 100 0 In te ns ity , a .u 706050403020 2 theta, degrees SnO2 SnO2 SnO2 SnO2 SnO2 60 50 40 30 20 10 6050403020 V2O5 V2O5 V2O5 V2O5 e f 40 30 20 10 In te ns ity , a .u 80706050403020 2 theta, degrees ZnO ZnO ZnO ZnO ZnO ZnO ZnO 160 140 120 100 80 60 40 20 In te ns ity , a .u 70605040302010 2theta, degrees ZrO2 ZrO2 ZrO2 ZrO2 g h Figure A7 XRD of single metallic oxides synthesized by sol-gel citric method (a: MnO2, b: Co3O4, c: NiO, d: CuO, e: SnO2 commercial, f: V2O5 commercial, g: ZnO, h: ZrO2) 0 10 20 30 40 50 60 70 200 250 300 350 400 450 500 Reaction temperature, oC C O c on ve rs io n, % CeO2 ZrO2 Co3O4 MnO2 NiO CuO SnO2 V2O5 ZnO Blank Figure A8 CO conversion of some single metallic oxides under deficient oxygen condition (O2/CO=1/4) Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 105 Annex 1.2.2 Characterization and catalytic activity of bi-metallic oxides 80604020 2 theta, degree before reaction after reaction SnO2 SnO2 SnO2 MnO2 MnO2 Figure A9 XRD patterns of MnO2-SnO2=4-6 before and after CO oxidation reaction in deficient oxygen (O2/CO=1/4) 0 10 20 30 40 50 60 200 250 300 350 400 450 500 Reaction temperature, oC C O c on ve rs io n, % MnO2 MnSn 8-2 MnSn 6-4 MnSn 4-6 MnSn 2-8 SnO2 Figure A10 CO conversion of MnO2-SnO2 in deficient oxygen condition (O2/CO=1/4) at different reaction temperatures 80604020 2 theta, degree before after MnO2 ZnO ZnO MnO2 MnO2 ZnO Figure A11 XRD pattern of MnO2-ZnO=5-5 before and after CO oxidation in deficient oxygen condition Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 106 Table A2 Specic surface area of MnO2-ZnO samples Sample MnO2 MnZn 9-1 MnZn 8-2 MnZn 7-3 MnZn 6-4 MnZn 5-5 MnZn 4-6 MnZn 3-7 ZnO SBET (m2/g) 5.61 6.27 23.78 21.66 14.52 23.62 32.17 22.34 13.62 0 10 20 30 40 50 60 200 250 300 350 400 450 500 Reaction temperature, oC C O c on ve rs io n, % MnO2 MnZn 9-1 MnZn 7-3 MnZn 4-6 MnZn 6-4 MnZn 3-7 ZnO Figure A12 CO conversion of MnO2-ZnO in deficient oxygen condition (O2/CO=1/4) at different reaction temperatures 0 20 40 60 80 200 250 300 350 400 450 500 Reaction temperature , oC C O c on ve rs io n, % MnO2 MnCo 9-1 MnCo 7-3 MnCo 5-5 MnCo 1-3 MnCo 1-9 Co3O4 Figure A13 CO conversion of MnO2-Co3O4 in deficient oxygen condition (O2/CO=1/4) at different reaction temperatures Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 107 80706050403020 2 theta, degrees before After Co3O4 Co3O4 Co3O4 MnO2 Figure A14 XRD patterns of MnO2-Co3O4=7-3 before and after CO oxidation reaction under deficient oxygen condition (O2/CO=1/4) a b Figure A15 SEM images of MnO2-Co3O4 =1-3 before (a) and after (b) reaction under deficient oxygen condition Table A3 CO conversion of some samples under sufficient oxygen condition (Figure 3.8) Temperature, oC MnCo 1-3 Co3O4 MnSn 4-6 MnO2 100 6 1.8 0 100 150 93 1.8 0 100 200 92.3 10.9 0 100 250 92.1 96 100 100 300 91.6 96.7 100 100 350 91.3 100 100 100 400 91.3 100 100 100 450 92.2 100 100 100 500 92.7 100 100 100 Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 108 Annex 2 The catalysts for simultaneous treatment of CO, C3H6 and NO Annex 2.1 The catalytic activity of bi-metallic oxides for simultaneous treatment of CO, C3H6 and NO 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature, oC C O c on ve rs io n, % Blank MnCo 1-3 MnSn 8-2 MnSn 9-1 a 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature, oC C 3H 6 c on ve rs io n, % Blank MnCo 1-3 MnSn 8-2 MnZn 9-1 b 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature, oC N O c on ve rs io n, % Blank MnCo 1-3 MnSn 8-2 MnZn 9-1 c Figure A16 CO conversion (a), C3H6 conversion (b) and NO conversion (c) of some bimetallic oxides in gas flow containing 4.35% CO, 7.06% O2, 1.15% C3H6, 1.77% NO Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 109 Annex 2.2 The catalytic activity of MnCoCe catalyst for simultaneous treatment of CO, C3H6 and NO Annex 2.2.1 MnO2-Co3O4-CeO2 with MnO2/Co3O4= 1/3 Table A4 CO conversion of MnCoCe catalyst with MnO2/Co3O4=1/3 in gas flow containing 4.35% CO, 7.65% O2, 1.15% C3H6, 0.59% NO (Figure 3.23a) Temperature, oC MnCoCe 1-3-0.17 MnCoCe 1-3-0.38 MnCoCe 1-3-0.75 MnCoCe 1-3-1.26 MnCoCe 1-3-1.88 100 0.49 98.40 99.6 99.58 99.63 150 2.80 98.50 99.68 99.60 99.61 200 98.71 98.42 99.56 99.67 99.54 250 98.73 98.60 99.59 99.64 99.55 300 98.75 98.67 99.73 99.66 99.41 350 98.77 98.46 99.62 99.62 99.48 400 98.81 98.44 99.77 99.75 99.51 450 98.85 98.28 99.83 100 99.4 500 98.86 98.33 99.91 100 99.48 Table A5 C3H6 conversion of MnCoCe catalyst with MnO2/Co3O4=1/3 in in gas flow containing 4.35% CO, 7.65% O2, 1.15% C3H6, 0.59% NO (Figure 3.23b) Temperature, oC MnCoCe 1-3-0.17 MnCoCe 1-3-0.38 MnCoCe 1-3-0.75 MnCoCe 1-3-1.26 MnCoCe 1-3-1.88 100 96.89 98.71 97.44 97.75 3.4 150 96.51 98.32 97.01 97.1 3.8 200 96.73 98.02 96.79 97.69 95.39 250 96.91 97.99 96.73 97.2 95.52 300 97.08 97.99 96.94 97.49 95.53 350 97.28 98.07 97.2 97.5 95.77 400 97.52 98.24 97.49 97.65 95.62 450 97.73 98.58 97.73 98.44 95.99 500 97.91 98.88 98.1 98.19 96.37 Annex 2.2.2 MnO2-Co3O4-CeO2 with different MnO2/Co3O4 ratio Table A6 CO conversion of MnCoCe catalysts in in gas flow containing 4.35% CO, 7.06% O2, 1.15% C3H6, 1.77% NO (Figure 3.24, Figure 3.26 a) Temperature, oC MnCoCe 1-3-0.38 MnCoCe 1-3-0.75 MnCoCe 7-3-1.11 MnCoCe 7-3-2.5 MnCoCe 7-3-4.29 100 2.67 96.7 0 0 0 150 4.37 96.17 0.72 1.59 0 200 85.00 96.30 87.84 92.11 94.86 250 85.98 94.97 86.75 96.80 95.20 300 86.82 95.27 86.35 91.09 98.19 350 87.40 94.81 86.73 88.70 99.31 400 87.60 94.65 86.47 88.54 100 450 90.36 93.46 85.80 88.16 99.23 500 91.41 94.21 86.45 97.12 99.80 Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 110 Table A7 C3H6 conversion of MnCoCe catalysts in 4.35% CO, 7.06% O2, 1.15% C3H6, 1.77% NO (Figure 3.24, Figure 3.26b) Temperature, oC MnCoCe 1-3-0.38 MnCoCe 1-3-0.75 MnCoCe 7-3-1.11 MnCoCe 7-3-2.5 MnCoCe 7-3-4.29 100 96.71 100 0 0 0 150 96.86 100 0 98.56 2.99 200 96.90 100 2.07 98.79 96.87 250 97.26 100 91.83 98.24 97.48 300 97.73 100 94.42 97.83 97.52 350 97.67 100 95.76 97.65 97.53 400 97.25 100 98.43 98.22 98.16 450 97.63 100 98.62 98.75 98.76 500 97.89 100 98.42 99.00 99.00 Table A8 NO conversion of MnCoCe catalysts in 4.35% CO, 7.06% O2, 1.15% C3H6, 1.77% NO (Figure 3.24, Figure 3.26c) Temperature, oC MnCoCe 1-3-0.38 MnCoCe 1-3-0.75 MnCoCe 7-3-1.11 MnCoCe 7-3-2.5 MnCoCe 7-3-4.29 100 81.44 62.11 0 0 0 150 85.89 63.54 0 48.95 0 200 90.75 66.042 0.13 50.04 54.31 250 93.38 70.56 24.11 62.32 60.38 300 99.77 75.17 27.10 71.98 66.22 350 100 82.10 42.88 75.98 73.14 400 100 99.06 54.28 80.34 75.76 450 100 92.00 74.83 83.12 78.79 500 100 99.65 85.12 100 84.03 Annex 2.2.3 Influence of aging condition on activity of MnCoCe catalysts Table A9 C3H6 conversion of MnCoCe 1-3-0.75 fresh and after aging in different conditions (Figure 3.35 a) Temperature, oC 0 1 2 3 4 5 100 97.44 0 1.96 3.1 0.39 3.58 150 97.01 40.68 1.86 2.47 85.6 1.19 200 96.79 65.31 94.48 95.01 90.02 98.74 250 96.73 97.02 94.88 95.46 90.61 98.74 300 96.89 93.72 95.32 95.62 91.63 98.77 350 97.2 97.74 95.12 95.83 92.17 97.61 400 97.49 97.91 95.46 96.05 93.86 97.96 450 97.73 98.21 95.86 96.56 95.09 98.15 500 98.09 98.09 96.63 97.31 96.24 98.62 Table A10 CO conversion of MnCoCe 1-3-0.75 fresh and after aging in different conditions (Figure 3.35 b) Temperature, oC 0 1 2 3 4 5 100 99.56 0 0 0 0 0 150 99.68 3.57 1.2 1.04 82.24 0 200 99.56 97.47 1.34 2.08 82.48 98.67 250 99.59 98.65 0.04 99.28 83.85 98.8 Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 111 300 99.73 97.89 98.86 99.56 87.33 99.01 350 99.62 98.01 99.35 99.78 88.85 98.69 400 99.77 98.57 99.78 99.84 91.83 98.8 450 99.83 99.03 99.03 99.34 95.09 98.84 500 99.1 99.32 99.45 99.58 97.83 98.96 Annex 2.2.4 Study on the improvement of catalytic activity of MnO2-Co3O4-CeO2 catalyst by addition of the fourth metallic oxides Table A11 CO conversion of catalysts based on MnO2, Co3O4, CeO2, BaO and WO3 in the gas flow containing 4.35% CO, 7.06% O2, 1.15% C3H6, 1.77% NO (Figure 3.41 a) Temperature, oC MnCoCe 1-3-0.75 15% BaO 10% BaO 5% BaO 15% WO3 5% WO3 100 97 0 1.86 6.79 6.79 2.35 150 96.17 1.92 3.18 6.03 6.03 1.74 200 96.28 88.50 95.11 92.99 92.99 2.22 250 94.97 88.64 91.84 92.38 92.38 95.73 300 95.27 88.46 88.04 92.25 92.25 94.96 350 94.81 91.46 87.30 92.84 92.84 94.98 400 94.65 90.00 87.29 90.91 90.91 94.40 450 93.46 92.05 87.17 91.40 91.40 92.79 500 94.21 92.36 90.51 92.47 92.47 92.95 Table A12 C3H6 conversion of catalysts based on MnO2, Co3O4, CeO2, BaO and WO3 in the gas flow containing 4.35% CO, 7.06% O2, 1.15% C3H6, 1.77% NO (Figure 3.41 b) Temperature, oC MnCoCe 1-3-0.75 15% BaO 10% BaO 5% BaO 15% WO3 5% WO3 100 100 0 96.49 8.89 8.89 0.42 150 100 2.00 96.21 0.11 0.11 0.56 200 100 82.85 96.16 94.89 94.89 93.29 250 100 83.13 96.23 95.45 95.45 93.96 300 100 85.18 96.67 96.04 96.04 94.48 350 100 88.72 97.07 96.42 96.41 97.00 400 100 90.49 96.42 97.37 97.37 97.50 450 100 90.20 96.79 100 100 97.90 500 100 91.14 96.94 100 100 98.87 Table A13 NO conversion of catalysts based on MnO2, Co3O4, CeO2, BaO and WO3 in the gas flow containing 4.35% CO, 7.06% O2, 1.15% C3H6, 1.77% NO (Figure 3.41 c) Temperature, oC MnCoCe 1-3-0.75 15% BaO 10% BaO 5% BaO 15% WO3 5% WO3 100 62.11 0 77.59 3.65 3.65 1.189 150 63.54 4.14 79.95 6.41 6.41 0.24 200 66.04 53.05 83.51 27.99 27.99 20.77 250 70.56 51.73 87.94 31.53 31.53 24.50 300 75.17 52.36 93.17 34.36 34.36 24.78 350 82.10 80.49 95.91 37.28 37.28 37.90 400 99.06 94.21 98.46 43.35 43.35 40.25 450 92.00 94.08 100 47.76 47.76 44.70 500 99.65 98.69 100 50.45 50.45 50.33 Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 112 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature, oC C O c on ve rs io n, % MnCoCe 7-3-2.5 10% CuO 50% CuO 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature, oC C 3H 6 c on ve rs io n, % MnCoCe 7-3-2.5 10% CuO 50% CuO 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature, oC N O c on ve rs io n, % MnCoCe 7-3-2.5 10% CuO 50% CuO Figure A17: Catalytic activity of MnCoCe 7-3-2.5 added CuO 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature, oC C O c on ve rs io n, % MnCoCe 7-3-2.5 10% ZnO 50% ZnO a Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 113 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature, oC C 3H 6 c on ve rs io n, % MnCoCe 7-3-2.5 10% ZnO 50% ZnO b 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature , oC N O c on ve rs io n, % MnCoCe 7-3-2.5 10% ZnO 50% ZnO c Figure A18: Catalytic activity of MnCoCe 7-3-2.5 added ZnO Annex 2.3 The catalytic activity of MnCoNi catalysts for simultaneous treatment of CO, C3H6 and NO Annex 2.3.1 The catalytic activity of MnCoNi catalyst with different MnO2/Co3O4 ratio 0 20 40 60 80 100 100 200 300 400 500 Reaction temperature, oC C O c on ve rs io n, % MnCoNi 2-3-3 MnCoNi 7-3-3 Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 114 0 20 40 60 80 100 100 200 300 400 500 Reaction temperature, oC C 3H 6 c on ve rs io n, % MnCoNi 2-3-3 MnCoNi 7-3-3 0 20 40 60 80 100 100 200 300 400 500 Reaction temperature, oC N O c on ve rs io n, % MnCoNi 2-3-3 MnCoNi 7-3-3 Figure A19 CO, C3H6 and NO conversion of catalyst MnCoNi 2-3-3 and MnCoNi 7-3-3 Annex 2.3.2 The catalytic activity of MnCoNi 7-3-3 catalyst added CeO2 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature, oC C O c on ve rs io n, % MnCoNi 7-3-3 5% CeO2 a Synthesize and investigate the catalytic activity of three-way catalysts based on mixed metal oxides for the treatment of exhaust gases from internal combustion engine Nguyen The Tien 115 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature, oC C 3H 6 c on ve rs io n, % MnCoNi 7-3-3 5% CeO2 b 0 20 40 60 80 100 100 150 200 250 300 350 400 450 500 Reaction temperature, oC N O c on ve rs io n, % MnCoNi 7-3-3 5% CeO2 c Figure A20 Catalytic activity of MnCoNi 7-3-3 and added 5% CeO2 sample

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