TW201328777A - 奈米金-銀承載於二氧化鈰觸媒之製法及其在去除空氣中一氧化碳之應用 - Google Patents
奈米金-銀承載於二氧化鈰觸媒之製法及其在去除空氣中一氧化碳之應用 Download PDFInfo
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- 239000003054 catalyst Substances 0.000 title claims abstract description 36
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 25
- 229910002091 carbon monoxide Inorganic materials 0.000 title claims abstract description 25
- 238000002360 preparation method Methods 0.000 title abstract description 3
- PQTCMBYFWMFIGM-UHFFFAOYSA-N gold silver Chemical compound [Ag].[Au] PQTCMBYFWMFIGM-UHFFFAOYSA-N 0.000 title description 7
- 239000010931 gold Substances 0.000 claims abstract description 34
- 229910052737 gold Inorganic materials 0.000 claims abstract description 31
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims abstract description 25
- 229910052709 silver Inorganic materials 0.000 claims abstract description 20
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims abstract description 19
- 239000004332 silver Substances 0.000 claims abstract description 19
- 238000000034 method Methods 0.000 claims abstract description 15
- 239000002245 particle Substances 0.000 claims abstract description 4
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 15
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 15
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical compound [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 claims description 14
- 239000012153 distilled water Substances 0.000 claims description 13
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 13
- 238000003756 stirring Methods 0.000 claims description 12
- 229910001961 silver nitrate Inorganic materials 0.000 claims description 7
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 claims description 5
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 claims description 5
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 4
- 235000011114 ammonium hydroxide Nutrition 0.000 claims description 4
- 238000001556 precipitation Methods 0.000 claims description 4
- 230000008021 deposition Effects 0.000 claims description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims 2
- 229910002092 carbon dioxide Inorganic materials 0.000 claims 1
- 239000001569 carbon dioxide Substances 0.000 claims 1
- 239000000203 mixture Substances 0.000 claims 1
- 230000003647 oxidation Effects 0.000 abstract description 6
- 238000007254 oxidation reaction Methods 0.000 abstract description 6
- DSRNAEXPGUGESR-UHFFFAOYSA-N [Ce].[Ag].[Au] Chemical compound [Ce].[Ag].[Au] DSRNAEXPGUGESR-UHFFFAOYSA-N 0.000 abstract 2
- 239000000243 solution Substances 0.000 description 14
- 238000006243 chemical reaction Methods 0.000 description 10
- 239000002253 acid Substances 0.000 description 6
- 238000006555 catalytic reaction Methods 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 3
- 239000007864 aqueous solution Substances 0.000 description 3
- 239000010970 precious metal Substances 0.000 description 3
- 239000002244 precipitate Substances 0.000 description 3
- 229910002701 Ag-Co Inorganic materials 0.000 description 2
- 230000010718 Oxidation Activity Effects 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- WOCIAKWEIIZHES-UHFFFAOYSA-N ruthenium(iv) oxide Chemical compound O=[Ru]=O WOCIAKWEIIZHES-UHFFFAOYSA-N 0.000 description 2
- 238000004448 titration Methods 0.000 description 2
- 238000005303 weighing Methods 0.000 description 2
- HEAMKOIGXQVULV-UHFFFAOYSA-N [O-2].[O-2].[Ce+3].[Au+3] Chemical class [O-2].[O-2].[Ce+3].[Au+3] HEAMKOIGXQVULV-UHFFFAOYSA-N 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- 238000000975 co-precipitation Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229910003455 mixed metal oxide Inorganic materials 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
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- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/66—Silver or gold
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- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
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- B01J37/031—Precipitation
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/864—Removing carbon monoxide or hydrocarbons
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
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Abstract
本發明揭示一種製備將奈米金及銀承載於二氧化鈰之觸媒方法,及一種在奈米金及銀承載於二氧化鈰之觸媒催化下,在空氣中一氧化碳與氧氣反應以去除一氧化碳之方法;其中金重量百分比是介於0.5%至5%,金及銀係依不同重量比例混合,金/銀重量比為0.1與1之間,承載之金和銀顆粒直徑為1與3奈米之間。本發明以含有金-銀/二氧化鈰觸媒在一氧化碳於空氣中,使用填充床反應器,以去除一氧化碳。
Description
本發明揭示一種製備奈米金-銀承載於二氧化鈰之觸媒方法,及一種在奈米金-銀承載於二氧化鈰之觸媒催化下,在空氣中一氧化碳與氧氣反應以去除一氧化碳之方法;其中金重量百分比是介於0.5%至5%,金及銀係依不同重量比例混合,金/銀重量比為0.1與1之間,承載之金和銀顆粒直徑為1與3奈米之間:本發明以含有金-銀/二氧化鈰觸媒在一氧化碳於空氣中,使用填充床反應器,以去除一氧化碳。
國內現有的專利有關金觸媒專利大部分都在一氧化碳氧化上的應用,並且並無使用金-銀/二氧化鈰的雙金屬觸媒,在100℃以下進行反應。一氧化碳氧化是使用貴重金屬觸媒如Pt,Au等[J. Power Sources第135卷(2004)第177頁至183頁;Journal of Power Sources,第165卷(2007)第353頁至358頁;Catalysis Letter第127卷(2009)第339頁至347頁],但昂貴的價格限制了貴金屬觸媒的發展,以金觸媒來說,通常要擔上3 wt.%以上的金,反應活性才會好。因此加入價格較低的金屬來提高活性是主要目標。而加入較低價格的銀改質金-二氧化鈰觸媒在此反應上有較好的活性,在貴金屬觸媒的改良方面,[Journal of Catalysis,第281卷(2011)第40頁至49頁]利用共沉澱法製備出Ag-Co雙金屬觸媒,進行不同溫度的鍛燒過後的CO氧化活性、選擇率及XRD研究,結果由XRD觀察指出,在鍛燒溫度為200℃時,Ag和Co會形成AgCoO2,此時的表面積為最大,而此經過鍛燒過的Ag-Co雙金屬觸媒其CO氧化活性是有因為Ag和Co會形成AgCoO2的關係而提高的。
國內目前有關金觸媒應用專利,公開號200613048揭示一種奈米金承載於氧化鈰觸媒之製法及其在去除氣體中一氧化碳的應用,美國專利5258340揭示一種混和金屬氧化物觸媒治法及其在去除氣體中一氧化碳的應用。由已公開專利中,未有如本發明所揭示利用奈米金及銀承載於二氧化鈰觸媒應用在一氧化碳氧化的方法。
本發明揭示一種製備將奈米金及銀承載於二氧化鈰之觸媒方法,及一種在奈米金及銀承載於二氧化鈰之觸媒催化下,在空氣中一氧化碳與氧氣反應以去除一氧化碳之方法;其中金及銀係依不同重量比例混合,金重量百分比是介於0.5%至5%,金/銀重量比為0.1與1之間,承載之金和銀顆粒直徑為1與3奈米之間。本發明以含有金-銀/二氧化鈰觸媒在一氧化碳於空氣中,使用填充床反應器,以去除一氧化碳。本發明的好處為用較少量的金,加入銀之後,可以有很高的活性。
以沉積沉澱法製備金-銀之雙金屬觸媒,以二氧化鈰作為負載的擔體,將金及銀依不同重量比例混合。
1.先稱取適量的二氧化鈰溶解於適量的蒸餾水中,以磁石攪拌之,並加熱至50至80℃之間任意溫度,並維持之;
2.再稱取適量的硝酸銀溶解於適量的蒸餾水中,將硝酸銀水溶液慢慢滴入二氧化鈰溶液中並攪拌2至8小時;
3.稱取適量的四氯金酸,將其溶解於蒸餾水中;
4.以氨水將步驟3之溶液酸鹼值控制在7至9,再將四氯金酸溶液慢慢滴入此溶液中,並同時控制鹼值在7至9,溫度維持在50至80℃之間任意溫度;
5.以磁石攪拌混合兩小時,維持酸鹼值在7至9,溫度50至80℃之間任意溫度;
6.將得到的沉澱物過濾,並以蒸餾水水洗多次,直到完全除去氯離子,再於50至150℃之間任意溫度烘乾;
7.將烘乾後的觸媒在80至20℃於空氣中煅燒,即生成Au-Ag/CeO2觸媒。
1. 製作金和銀重量比為5:5的觸媒。先稱取2.97g二氧化鈰溶解於400ml蒸餾水中,以磁石攪拌之,並加熱至65℃,並維持之;
2.再稱取0.015g硝酸銀溶解於5ml蒸餾水中,將硝酸銀水溶液慢慢滴入二氧化鈰溶液中並攪拌兩小時;
3.稱取0.8ml的0.0125g Au/ml四氯金酸溶液,將其加入7.2ml蒸餾水稀釋十倍;
4.以0.1M氨水將步驟3之溶液酸鹼值控制在8±0.2,再將四氯金酸溶液以每分鐘5-20毫升之間任意速率滴入此溶液中,並同時控制鹼值在8±0.2,溫度維持65℃;
5.滴定完成後以磁石攪拌混合兩小時,維持酸鹼值在8±0.2,溫度65℃,使其反應完全;
6.將得到的沉澱物過濾,並以60℃之蒸餾水水洗多次,直到完全除去氯離子,再於80℃烘乾16小時;將烘乾後的觸媒在180℃於空氣中煅燒4時,即生成Au-Ag/CeO2適當比例的粉末。
1.製作金和銀重量比為5:5的觸媒。先稱取2.97g二氧化鈰溶解於400ml蒸餾水中,以磁石攪拌之,並加熱至65℃,並維持之;
2.再稱取0.015g硝酸銀溶解於5ml蒸餾水中,將硝酸銀水溶液慢慢滴入二氧化鈰溶液中並攪拌兩小時;
3. 稱取0.8ml的0.0125g Au/ml四氯金酸溶液,將其加入7.2ml蒸餾水稀釋十倍;
4. 以0.1M氨水將步驟3之溶液酸鹼值控制在8±0.2,再將四氯金酸溶液以每分鐘5-20毫升的速率滴入此溶液中,並同時控制鹼值在8±0.2,溫度維持65℃;
5. 滴定完成後以磁石攪拌混合兩小時,維持酸鹼值在8±0.2,溫度65℃,使其反應完全;
6. 將得到的沉澱物過濾,並以60℃之蒸餾水水洗多次,直到完全除去氯離子,再於80℃烘乾16小時;將烘乾後的觸媒在350℃於空氣中煅燒4時,即生成Au-Ag/CeO2適當比例的粉末。
1. 將觸媒Au-Ag/CeO2,置於填充床反應器內,進行在空氣中氧化一氧化碳的反應,以固定床反應器進行反應,一氧化碳濃度在5 vo;.%至100 ppm之間;
2. 控制空間流速在10至10,000 h-1,在溫度25至200℃之間任意溫度下通入反應器中;可將一氧化碳完全氧化。
1. 將0.1g的Au-Ag(5:5)/CeO2觸媒置於直立式填充床反應器內,進行在空氣中氧化一氧化碳的反應,以固定床反應器進行反應;
2. 控制流量為每分鐘50毫升,在不同溫度下通入反應器中;
3. 一氧化碳濃度由氣相層析儀偵測得之。
1. 將0.1g的Au-Ag(5:5)/CeO2觸媒置於直立式填充床反應器內,進行在空氣中氧化一氧化碳的反應,以固定床反應器進行反應;
2. 控制流量為每分鐘50毫升,在不同溫度下通入反應器中;
3. 一氧化碳濃度由氣相層析儀偵測得之。
Claims (2)
- 一種製備將奈米金及銀承載於二氧化鈰之觸媒方法,其包括:以沉積沉澱法製備之金和銀承載於二氧化鈰之觸媒,金與銀混合之重量比例在0.01至2之間,金重量百分比是介於0.5%至5%,其特徵是將硝酸銀溶液以沉澱沉積法與二氧化鈰混合後,於50℃至80℃間攪拌2至8小時,再以沉積沉澱法將金溶液滴入上述溶液中,以氨水控制酸鹼值在5至9間及維持溫度在50℃至80℃之間並持續攪拌,維持1至10小時後,以50℃至80℃之間蒸餾水洗,50℃至150℃之間烘乾8至24小時,在120℃至240℃之間煅燒2至8小時,承載之金和銀顆粒直徑為1與3奈米之間。
- 一種去除空氣中含有一氧化碳的方法,其係以含有奈米金及銀承載於二氧化鈰觸媒,在空氣中於25℃至200℃間反應,使一氧化碳氧化成二氧化碳,其中奈米金及銀承載於二氧化鈰觸媒為申請專利範圍第1.項所製造之觸媒。
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