ܴཥࣽמεᏢਠϣᚒࣴزीฝԋ݀ൔ
ीฝᜪձǺ Һ୍ࠠीฝ ӝࠠीฝ
ɍঁΓीฝ
ीฝጓဦǺNVTU.ϯ.7
Չය໔Ǻ104 ԃ 1Д 1 ВԿ 104 ԃ 9 Д 30В
ीฝЬΓǺഋճம
ीฝୖᆶΓǺሎϡ
ೀБԄǺϦ໒ܭਠᆛ।
ՉൂՏǺϯᏢπำᆶࣽמس
ύ҇୯ 104 ԃ 9 Д 30 В
Ԯᅹబуణ਼ϯႇᗋচ਼ϯේޜԦࢉނϐࣴز
The Study of NO Air Pollutant Reduction by KOH Contained
Abstract
A bamboo activated carbon is made from the waste bamboo chopsticks in this study. The bamboo chopsticks are carbonized in 400к at the beginning, then followed by activated in 750к at the atmosphere of CO2 to prepare the bamboo
activated carbon (BAC). Followed, the BAC is acid treated by 6N hydrogen chloride. After that, the BACs will be impregnated separately in KOH solutions of 0, 3, 6, 10 and 20wt% for one hour. Finally, after filtration, the BACs doping with KOH are dried in conditions of 30, 60 and 105к separately. The prepared BAC catalysts will be used for the NO conversion reaction.The function groups on the surfaces of the BAC catalysts are also measured by FT-IR. The surface properties of the BAC catalysts are also analyzed by SEM and BET. The elemental analysis of the BAC catalysts is analyzed by EDS. After all, the NO conversion characteristics of the BAC catalysts are tested in the conditions with 3%O2and without O2 at the temperature
range 30-180кto investigate the effects of doping KOH. The BAC catalysts are also tested through the thermo gravimetric analysis (TGA) to study the interrelations between the reaction temperature and thermal gravity.
The FT-IR tests show that the intensity of function groups is decreased in the surface of BAC catalysts which are doping with KOH. The BET tests of the BAC catalysts adding KOH indicate that the specific surface areas are also decreased significantly. Both of the above two effects revealing that there exist the competitions between the NO oxidation reaction by KOH and the NO reduction reaction by activated carbon. The NO conversion experiments in the atmosphere of 3% O2and the
temperature above 90к show that the NO conversion of BAC(30к, 6%KOH) is higher than the BAC without KOH. The NO conversion of BAC(30к, 6%KOH) reaches 80% in the atmosphere of 3%O2and 60к. But, under the atmosphere without
oxidation, all the experiments of the BAC catalysts with KOH indicate that the NO conversions are lower than that without KOH. Finally, the 36hrs life duration tests in 3%O2 and 180к show that the NO conversions of the BAC catalyst with KOH is
very close to that without KOH.
KeywordsΚBamboo carbon, acid treatment, KOH, low temperature NO conversion
ǵق
1.1ᆣፕ ӧࣽמวِೲޑжޗǴΓॺޑғࢲВᅌߡճǴғࢲНྗΨᒿϐගଯǶ ՔᒿԶٰޑࢂπቷǵεኴǵؓᐒًኧໆຫٰຫӭǴ௨ܫεໆޑྟၰϷቲ٬ள ᕉნᎁڙԡࢉǶӢԜӵՖफ़եޜԡࢉޑวғаϷ෧ϿჹᕉნޑઇᚯࢂҞШࣚ Ӛ୯ᜢݙޑᚒǶ πቷ௨ܫޑྟၰکؓᐒً௨ܫޑቲύх֖Αේ਼ϯނ(NOx)Ϸ౷਼ϯ ނ(SOx)Ǵ೭٤ϯӝނࢂԋለߘ(acid rain)کӀϯᏢྟᜦ(photochemical smog)ޑ Ьाٰྍ[ቅǴ1998]Ƕේ਼ϯނࢂԋૌ਼ޑ០ނ፦ϐǴεύේ਼ϯނа NOǵNO2ǵNO3ϷN2OࠠᄊӸӧǴቲύ܌ᒏޑේ਼ϯނ(NOX)ࢂࡰNOϷNO2ǴNOӧεύ਼ϯԋNO2ǴԶNO2ڙӀྣࡕǴΞϩှӣNOϷ਼চ
ϯᏢϸᔈԋ਼߄य़ϯӝނǶԜѦǴᅹ-਼߄य़୷ՏޑԋόࢂٰԾܭᆶ਼ ޑϸᔈǴҭёҗᆶ਼ϯ܄ᡏ(ૌ਼ǵේ਼ϯނǵΒ਼ϯᅹ...)܈਼ϯ܄ྋ న(ฮለǵၸ਼ϯణ...)ౢғǶᅹޑ਼߄य़ፄӝނϐ܄፦ϷኧໆЬाࢂڙځК ߄य़ᑈǵᗭಈಈ৩ǵԪϩ֖ໆǵྕࡋǵϷᅹϯำࡋ܌ቹៜ[මǴ2002]Ƕ
җܭࢲ܄ᅹ༹ሽϷᓬຫޑ่ᄬ܄Ǵ߈ԃٰаࢲ܄ᅹᇙբ൞٠ҔӧNOᗋ চϸᔈሦୱڙډቶݱޑࣴزȘIllan-Gomez et al., 1996; Zhuet al., 2000]Ƕձࢂа ࢲ܄ᅹࣁᏼᡏਔǴၸለೀǴёаቚуځ߄य़ޑለ܄਼֖۔ૈ୷Ǵගϲᡏ ޑϯࢲ܄Ƕ 1.2ЎЎӣ៝ 1.2.1ࢲ܄ᅹᙁϟ ࢲ܄ᅹޑЬाԋϩࣁᅹ(C)ǴӕਔΨ֖ԖٰԾচ܈ࢂబуނޑϿໆ܈༾ໆ ϐคᐒނ፦Ǵࢲ܄ᅹ(Activated Carbon)ࣁӭϾ܄ᅹᡏޑӝᆀǶᇙБݤࣁஒ֖ᅹ ނ፦ᅹϯ(carbonization)Ǵӆၸࢲϯ(activation)ԶளǶ ΥӸܭԾฅᕉნύϐ֖ᅹԋϩၨӭޑǵǵނϐނ፦Ǵၸೀ ࡕ֡ૈԋࢲ܄ᅹǶ߈ԃٰբࣁࢲ܄ᅹচޑٰྍ׳ࣁӭኬϯǶҞ٬Ҕϐ চЬाԖǺ 1.ނБय़ǺٯӵЕǵዿෘǵྲྀηෘǵނମᓝǶ 2.ΓπӝԋচБय़ǺΓᠼᆢǵᆫЧᐋ✊ǵᐎጤǶ 3.ҡϷᐯБय़Ǻขࣅǵᛅߙǵݝྡǵҡݨᇃᚖූ෦Ƕ Ҟϯޑࢲ܄ᅹচаЕǵྲྀηෘکྡࣁЬǴӧᒧচਔǴᓬ ӃԵໆޑྗ߾х֖Ԫҽ֖ໆǵሽǵᓯӸϐტڮаϷڗளϐᜤܰ[ጰΓǴ 1993]Ƕ 1.2.2ࢲ܄ᅹϐᇙ ࢲ܄ᅹࢂϾሜᄬϷК߄य़ᑈၨεޑᅹનǴӢԶቶݱᔈҔܭπ ٮբ֎ߕϷ൞ၩᡏ٬ҔǴځٰྍӧԾฅᕉნύӸӧϐނϷނǴѝा ڀଯ֖ᅹໆёࣁᇙࢲ܄ᅹޑচǶҞࢲ܄ᅹаྡǵЕکྲྀηෘന ӭǴځύΞӢྡӧԾฅࣚޑᙒໆᙦǴЪሽե༹ǴӢԜԖӭኧޑࢲ܄ᅹࢂҗ ྡ܌ᇙԶԋǴҗܭྡҁي֎ߕϷ߄य़ࢲ܄ό٫ǴӢԜሡаᅹϯ(carbonization) Ϸࢲϯ(activation)ၸำٰ㽲уځ֎ߕૈΚǶᅹϯᆶࢲϯޑၸำϩॊӵΠǺ 1.ᅹϯ ᅹϯǴᙁൂޑۓကࣁǺԖᐒϯӝނᙖҗǴᙯඤᡂԋᅹ[Lewis, 1982]ǶΞᆀ ࣁှ(pyrolysis)ǶѬࢂࡰӧආ܄ᡏύǴҔଯྕஒଯϩηނ፦ύޑߚᅹচη (ణǵ਼ǵේǵ౷)Ǵаචวނ(gas)کขݨ(tar,liquid)ԄញрǶߚᅹচηញрࡕǴ
วғӧ༾ϾύǶᗨฅύϾᆶѮϾӧࢲ܄ᅹޑϾࢰ่ᄬύ܌՞ޑКٯၨϿǴՠ ༾ϾεӭϩթӧύϾᆶѮϾϐύǴӢԜ֎ߕނ፦ѸၸύϾᆶѮϾωૈᘉ ණԿ༾ϾύǴӵკ1.1܌ҢǴ܌аύϾᆶѮϾӧ֎ߕำׇύҭתᄽΑ࣬ख़ा ޑفՅǶ კ 1.1 ࢲ܄ᅹϣᄬკ[Rodriguez-Reinoso, 1998] 1.2.4 ࢲࢲ܄ᅹϐ۔ૈ୷ ࢲ܄ᅹҗᜪ՟ҡᏀ܈ቫᄬޑཱུ༾λ่܌ಔԋǴ٠֖ࡐӭ่҃ᆄޑ ᜔य़Ǵځ߄य़Ԗεໆаࢲ܄ణ܈਼֖୷ࣁЬޑ߄य़۔ૈ୷Ǵ೭٤߄य़۔ૈ୷ӭъ ჹ߄य़֎ߕϐ܄Ԗ܌ቹៜǶ[Hall, 1992]วᇙࢲ܄ᅹޑࢲϯၸำύౢғ۔ ૈ୷Ǵ܈ᙖҗ਼ޑϯᏢ֎ߕԶғԋǶ[Park, 2001]ᇡࣁӧᅹϯ܈ࢲϯྕࡋܭ800ʚ аΠਔǴ߄य़਼֖۔ૈ୷όᛙۓǴԋᡵ܄۔ૈ୷ǴԶࢲ܄ᅹϐለ܄߄य़܄፦ Ьाࣁለ܄۔ૈ୷܌Ꮴठ[Boehm, 1994]Ƕለ܄۔ૈ୷Ξаcarbonylǵcarboxylǵ phenolicǵhydroxylǵlactoneϷquinone۔ૈ୷ࣁЬǴ࣬ၨܭለ܄۔ૈ୷Ǵᡵ ܄۔ૈ୷ၨคܴዴೕۓǴ೯த่ᄬύԖᜪ՟chromeneϷpyroneޣջឦܭᡵ܄۔ ૈ୷[Tomon et al., 1996]ǶӧࢌۓྕࡋΠǴ߄य़਼֖۔ૈ୷ញܫрCO2܈
COځύᅿᡏǴΨёૈӕញܫрCO2کCOǶ߄य़਼֖۔ૈ୷ޑғԋё
კ 1.2 ࢲ܄ᅹ߄य़ёૈޑ਼֖ለ܄۔ૈ୷[Boehm, 1994]
1.2.5ࢲࢲ܄ᅹ൞ନ NO ϐϸᔈ ٬Ҕࢲ܄ᅹ൞ޑNO ᗋচϸᔈΞёϩࣁబу NH3բࣁᗋচᏊᆶคబуNH3 ٿᅿǴځύబуΑ NH3բࣁᗋচᏊޑࢲ܄ᅹ൞ନ NO ϸᔈǴځЬाϸᔈБำ Ԅᆶޑ SCR ݤ࣬ӕǴคబу NH3ޑࢲ܄ᅹ൞ନ NO מೌҗܭࢲ܄ᅹёӕ ਔתᄽ൞ϷᗋচᏊޑفՅǴځϸᔈᆶ SCR ϸᔈԖᡉޑόӕǶ คబу NH3բࣁᗋচᏊޑࢲ܄ᅹନ NO מೌǴёᗉխᓯӸޑӼӄ܄аϷ ຽණܭቲύԋΒԛԦࢉୢᚒǴӢԜڙډᏢޣৎॺޑख़ຎǴӧԜᜪϸᔈ ύǴࢲ܄ᅹΨתᄽᗋচᏊޑفՅ٬ NO ᗋচǴԶځҁي߾਼ϯԶញр CO2
Ϸ CO ᡏǶਥᏵ[Khristova et al., 1998]Ϸ[Mehandjiev et al., 1996]ޑࣴزǴӧ ค NH3ᕉნΠନ NO ޑϸᔈё߄ҢࣁǺ ads s s g C C NO NO( ) ( ) o ( )[ ] (1) ] [ ] [ 2( ) ( ) ) ( NO N C O Cs ads o g s (2) Զӧ༾਼ޑݩΠǴO2ᆶࢲ܄ᅹϸᔈԶញр਼ϯᅹ(CO)ǴԶ CO ڀ ԖᗋচᏊޑਏ݀ёߦ NO ޑᗋচǺ
CO
O
C
2
2
2o
(3) 2 2N
CO
NO
CO
o
(4) ॊޑϸᔈᗺрΑ NO ᗋচԶԋЬाౢނࣁ N2Ϸ CO2ޑЬाϸᔈǶ NO ޑᗋচϸᔈ٠ୖԵ Illan-Gomez Γ[1996]ޑࣴزёޕǴӧค਼Ϸค ޑᕉნΠ NO ޑᗋচϸᔈᐒᄬࢂၸ NO ֎ߕ/ᗋচϸᔈǵ਼ሀǵаϷౢ ނಥߕϸᔈΟঁᡯԶֹԋޑǺ NO ֎ߕ/ᗋচϸᔈǺ 2 f2NO
2C
O
N
2C
o
(5) C(O) O C l (ё) (6) * f 2 C CO 2C(O)o (7) 2 * f 2NO 2C O N 2C o (8) ॊፏԄύǴCf ж߄Ծҗᅹࢲ܄୷Ǵ(5)Ԅёှញࢲ܄ᅹ൞ӧեྕਔޑ NO ᗋচϸᔈǴஒ Cf਼ϯࣁ C-OǶྕࡋᅌϲଯਔǴ่ӝܭ C-O ύޑ਼ё ӧ ࢲ ܄ ᅹ ൞ ߄ य़ Չ ౽ Զ ԋ ߄ य़ ᅹ ਼ ύ ໔ ނ C(O)(Carbon-oxygen surface intermediate)Ǵёҗ(6)Ԅ߄ҢǶӧౢނಥߕၸำύǴC(O)ёՉϩှϸ ᔈ(7)ԄԶԋ CO2Ϸཥᅹࢲ܄୷ Cf*(Nascent carbon active site)Ǵཥᅹࢲ܄୷ӆᆶ NO ϸᔈ((8)Ԅ)ஒځᗋচࣁ N2ЪΞԋ C-OǴӵԜёុޑஒ NO ᗋচ ౢނಥߕϸᔈǺ
ࣁ N2٠ញܫр CO2Ƕॶளݙཀޑࢂॊ C-O ߄य़਼ϯނ٠ό߳ज़ܭԾϸᔈ
ύౢғǴҭёҗࢲ܄ᅹᇙၸำ܈ࢂ൞Ⴃ਼ϯၸำԶளډǶ
Ο
ΟǵࣴزБݤ
ҁࣴزࣁӧ 400ʚϐᕉნΠஒϪപԋऊ 5 ϦϩߏࡋޑԮࢤᅹϯǴӆճҔΒ ਼ϯᅹӧࢲϯྕࡋ 750ʚΠࢲϯᇙԋԮᅹࢲ܄ᅹǴฅࡕ٬Ҕ 6N ᐚࡋϐᡶለНྋ నՉለೀගଯځК߄य़ᑈǴനࡕӆၸόӕख़ໆК(3%ǵ6%ǵ10%ǵ20%) ϐణ਼ϯႇНྋనೀࡕǴ٠ӧόӕྕࡋ(30ʚǵ60ʚǵ105ʚ)ΠଳᔿǶ ځჹ NO ѐନϸᔈϐਏ݀Ǵϩձӧค਼Ϸ 3%਼ޑϸᔈచҹΠѐନ਼ϯේޜ ԦࢉނǶӧჴᡍၸำύǴନΑҔډᇙഢ൞Ϸෳ၂൞ҔޑᡏѦǴќᗋ௦Ҕ ൞ϸᔈෳ၂းǵේ਼ϯނϩሺǵख़ϩሺаϷК߄य़ᑈෳۓሺഢٰ Չ൞܄ૈޑෳ၂ᆶໆෳǶаΠ൩ҁჴᡍ܌٬ҔϐᡏǵሺᏔഢǵԮᅹ൞ϐ ᇙഢБݤǵ൞܄ૈෳ၂БݤϷሺᏔϩϩॊӵΠǺ 3.1 ჴᡍഢ 3.1.1 ᛰࠔ ҁࣴز܌٬ҔޑᛰࠔନԮᅹࣁԾᇙϐѦځᎩࣣࣁ၂ᛰભᛰࠔǴϩձ௶ॊӵ ΠǺ1. ԾᇙԮᅹ(Bamboo Activated carbon)Ǵಈ৩:0.15~0.42mm
2. ᡶለ(Hydrochloric acid)Ǵᐚࡋ 12N(EP ભ)ǴΦᛰࠔ
1. ଯྕуǺႝηуԄᆅރǴߏ 28cmǴϣ৩ 3cmǶ 2. ύޜҡमϸᔈᆅǺߏ 45cmǴϣ৩ 4mmǴҔа൞Ƕ 3. ᡏ፦ໆࢬໆڋᏔǺKD4000 / 4CH ࠠǴҔаڋᡏࢬໆǶ 4. ᡏ፦ໆࢬໆीǺ3 ЍǶ 5. ଽྕࡋᡉҢीǺଽࣁ K typeǴߏ 40cmǴѦ৩ 2mmǴҔаໆෳϸᔈ ᆅϣϐჴሞϸᔈྕࡋǶ
კ 3.2 ᡏ፦ໆࢬໆڋᏔ
კ 3.4 ᡏ፦ໆࢬໆी
3.2.1.3ᐨᐨѨीᆉ
ᐨѨ(Burn off rate)=ȴ(WiɡWf) / Wiȵ×100%
WiǺinitial bamboo weight ߃ۈނϐଳख़
WfǺfinal carbon weight ᐨᇙԋࠔϐଳख़
3.2.1.4 Ԯᅹለೀ ၸࣴᑃᑔϩϐಈރԮᅹ(0.15~0.42mm)ሡа 105ʚϐጃଳ 1 λਔǴଳ ࡕஒځа፦ໆК 1:5 КٯΕ 6N ᐚࡋϐᡶለНྋనύ٠аᅶҡᠳ 24 λਔǴ ӆՉᠳНࢱ(ࢱԿᘠనεܭ pH 5)ǴௗஒНࢱࡕಈރԮᅹа 105ʚଳǴ ଳࡕीᆉځለೀཞѨໆ(ـკ 3.7)ǶለೀࡕϐԮᅹа BAC(6N HCl)ᆀϐǶ კ 3.7 Ԯᅹለೀϐࢬำკ 3.2.1.5 ለೀϐԮᅹబуణ਼ϯႇ ၸለೀࡕޑԮᅹࢲ܄ᅹӃа 105ʚϐጃଳ 1 λਔǴଳࡕΕόӕ ख़ໆК(3%ǵ6%ǵ10%ǵ20%)ޑణ਼ϯႇНྋనύ٠аᅶҡᠳ 1 λਔǴၸᘠ ࡕϩձӧόӕྕࡋ(30ʚǵ60ʚǵ105ʚ)ΠଳǴଳࡕीᆉځख़ໆቚуໆ(ـკ 3.8)Ƕ 3%KOH Нྋనೀ٠ӧ 30ʚϐΠଳϐԮᅹа BAC(30ʚ 3% KOH)Ǵ ܭᜪǶ
Ԯᅹಈଳ 1 λਔ 105к
፦ໆК 1:5 КٯΕ 6N ᡶለНྋనύǴᠳ 24 λਔ
კ 3.8 ለೀԮᅹబуణ਼ϯႇϐࢬำკ
3.2.2 ख़ϩሺ(TGA)
3.2.3 ഡഡҥယᙯඤआѦጕӀሺ(FT-IR)
კ 3.11 JSM-6700 ࠠඔԄႝηᡉ༾᜔ 3.2.5 КК߄य़ᑈϩሺ(BET) BET Ͼሜϩሺ(SA 3100)ࣁኬࠔӧ 77K ޑྕࡋΠǴ٬Ҕ N2Չྕ֎ಥ ߕǴߡёளޕځϾሜ܄ǶෳໆஒኬࠔܫΕ 130ʚጃύଳᔿԿ႖ВǴӆஒኬ ࠔΕ U ࠠኬࠔᆅ٠ӼးܭሺᏔǴӆճҔухஒኬࠔᆅуԿ 210ʚ٠ܜ ޜ٬ᆅύᓸΚեܭ 10-4 torrǴᙖԜନѐԮᅹύූᎩНϩϷචวނ፦Ǵӆஒኬࠔᆅ ܭనᄊේఏύǴ٬ځᆢӧ 77K եྕΠǴ೯Ε N2ࡕՉෳໆǶෳໆֹԋࡕё
ளډࢲ܄ᅹϐ BET К߄य़ᑈ(SP)Ǵҁࣴز܌٬ҔޑሺᏔࢂऍ୯ Beckman Coulter
Ϧљ܌ᇙޑ SA 3100 К߄य़ᑈϷϾሜϩሺǶ(კ 3.12)
3.2.6 ൞܄ૈෳ၂ ҁࣴز௦ҔڰۓԄ൞ϸᔈෳ၂းٰՉ൞ନ NO ܄ૈෳ၂Ǵځϸᔈ ෳ၂းϷෳ၂ᡯϩॊӵΠ: 3.2.6.1 ϸᔈෳ၂း ஒଞჹለೀԮᅹϷለೀࡕబуణ਼ϯႇϐԮᅹӧค਼Ϸ 3%਼చҹΠ Չ NO ᗋচϸᔈ܄ૈෳ၂Ǵ௦ҔڰۓԄ൞ϸᔈෳ၂းໆෳ൞܄ૈǴϸ ᔈ٬Ҕޑᡏ 2000ppm NO in Heǵ8% O2in HeϷ He ࣣҗଯᓸᡏᒳ܌ගٮǴ
(a)6N HCl(BAC) (b) 30к 3% KOH(BAC)
(c) 30к 6% KOH(BAC) (d) 60к 6% KOH(BAC)
(e) 105к 6% KOH(BAC) (f) 30к 20% KOH(BAC)
(a)6N HCl(BAC) (b) 30к 3% KOH(BAC)
(c) 30к 6% KOH(BAC) (d) 60к 6% KOH(BAC)
(e) 105к 6% KOH(BAC) (f) 30к 20% KOH(BAC)
(a)6N HCl(BAC) (b) 30к 3% KOH(BAC)
(c) 30к 6% KOH(BAC) (d) 60к 6% KOH(BAC)
(e) 105к 6% KOH(BAC) (f) 30к 20% KOH(BAC)
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