JP7302942B2 - 有機ガス低減装置および有機ガス低減方法 - Google Patents
有機ガス低減装置および有機ガス低減方法 Download PDFInfo
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- JP7302942B2 JP7302942B2 JP2017032542A JP2017032542A JP7302942B2 JP 7302942 B2 JP7302942 B2 JP 7302942B2 JP 2017032542 A JP2017032542 A JP 2017032542A JP 2017032542 A JP2017032542 A JP 2017032542A JP 7302942 B2 JP7302942 B2 JP 7302942B2
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- Prior art keywords
- gas
- oxidation catalyst
- copper
- support
- organic gas
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- NFCRBQADEGXVDL-UHFFFAOYSA-M cetylpyridinium chloride monohydrate Chemical compound O.[Cl-].CCCCCCCCCCCCCCCC[N+]1=CC=CC=C1 NFCRBQADEGXVDL-UHFFFAOYSA-M 0.000 description 2
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- YEOCHZFPBYUXMC-UHFFFAOYSA-L copper benzoate Chemical compound [Cu+2].[O-]C(=O)C1=CC=CC=C1.[O-]C(=O)C1=CC=CC=C1 YEOCHZFPBYUXMC-UHFFFAOYSA-L 0.000 description 2
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- CMRVDFLZXRTMTH-UHFFFAOYSA-L copper;2-carboxyphenolate Chemical compound [Cu+2].OC1=CC=CC=C1C([O-])=O.OC1=CC=CC=C1C([O-])=O CMRVDFLZXRTMTH-UHFFFAOYSA-L 0.000 description 2
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- WFIPUECTLSDQKU-UHFFFAOYSA-N copper;ethyl 3-oxobutanoate Chemical compound [Cu].CCOC(=O)CC(C)=O WFIPUECTLSDQKU-UHFFFAOYSA-N 0.000 description 2
- JHIVVAPYMSGYDF-UHFFFAOYSA-N cyclohexanone Chemical compound O=C1CCCCC1 JHIVVAPYMSGYDF-UHFFFAOYSA-N 0.000 description 2
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- SRWMQSFFRFWREA-UHFFFAOYSA-M zinc formate Chemical compound [Zn+2].[O-]C=O SRWMQSFFRFWREA-UHFFFAOYSA-M 0.000 description 1
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
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Description
また、農産物からは熟成作用を有するエチレンが放出され、自身の熟成を進行させている。そのため、温度、湿度を一定に保つとともにこのエチレンガス濃度を低減することが、鮮度を長期間保持するために有効であるとされている。
また、光触媒を用いた鮮度保持装置では、触媒が作用するためには紫外光もしくは可視光が必要であるが、一般的に貯蔵中の保管庫は照明を点けないため、当該装置には触媒に照明が必要となり、構造が複雑になるとともに照明のための電力が余分に必要となる。
[1] 通気性を有し、その表面にメソ孔を有する膜状支持体が形成されている部材と、前記膜状支持体に被処理気体を供給する気体供給部とを備え、
前記膜状支持体のメソ孔において白金、パラジウムの単体およびこれらの酸化物からなる群から1種または2種以上選択される物質を含む酸化触媒粒子が担持されており、前記膜状支持体に供給された被処理気体中の有機ガスを酸化することを特徴とする有機ガス低減装置。
[2] 前記被処理気体中に含まれる有機ガスがエチレンであることを特徴とする[1]に記載の有機ガス低減装置。
[3] 前記気体供給部が非処理気体を膜状支持体に送風する送風機構を有しており、前記送風機構による送風の空間速度が10,000/h以上150,000/h以下であることを特徴とする[1]または[2]に記載の有機ガス低減装置。
[4] 前記部材のさらに空気流通方向上流側に配置される抗菌性、防カビ性、抗ウイルス性のうち少なくとも一つを有する化合物を担持する部材をさらに備えることを特徴とする[1]から[3]のいずれか一つに記載の有機ガス低減装置。
[5] 前記膜状支持体の膜厚が50nm以上1000nm以下であることを特徴とする[1]から[4]のいずれか一つに記載の有機ガス低減装置。
[6] 前記膜状支持体がSiO2で形成されていることを特徴とする[1]から[5]のいずれか一つに記載の有機ガス低減装置。
[7] 前記メソ孔のBET法で測定した平均孔径が2nm以上10nm以下であることを特徴とする[1]から[6]のいずれか一つに記載の有機ガス低減装置。
[8] 前記酸化触媒粒子の平均粒径が1nm以上10nm以下であることを特徴とする[1]から[7]のいずれか一つに記載の有機ガス低減装置。
[9] メソ孔を有し、当該メソ孔内に白金、パラジウムの単体およびこれらの酸化物からなる群から1種または2種以上選択される物質を含む酸化触媒粒子を担持している膜状支持体に被処理気体を供給して拡散させ、当該気体に含有される有機ガス濃度を低減させることを特徴とする有機ガス低減方法。
図1は本実施形態の有機ガス低減装置の概要を示す図である。図2、図3は本実施形態に係る白金、パラジウムの単体およびこれらの酸化物からなる群から1種または2種以上選択される物質を含む酸化触媒粒子(以下、単に酸化触媒粒子という場合もある)が担持された膜状支持体を有する部材の概要を示す図である。なお、図面において、実線の矢印は空気の移動方向を表し、また、破線の矢印は空気の酸化触媒層33における拡散を表す。
本実施形態の有機ガス低減装置100は、大気中などの微量有機ガスを酸化して、例えば青果物や花卉の生育に良好な大気状態を提供するために使用できる装置であり、通気性を有し、その表面にメソ孔37を有する膜状支持体34が形成されている部材30と、膜状支持体34に被処理気体を供給する気体供給部10とを備え、膜状支持体34のメソ孔37において酸化触媒粒子が担持されており、膜状支持体34に供給された被処理気体中の有機ガスを酸化する。なお、以下の説明においては酸化触媒粒子が担持されている膜状支持体34を酸化触媒層33とも称す。被処理気体が気体供給部10によって当該酸化触媒層33に供給されて拡散浸透することにより、非処理気体に含有する有機ガス成分が酸化触媒層33中の酸化触媒粒子によって酸化される。
本実施形態の有機ガス低減装置100によれば、酸化触媒層33の体積や担持される酸化触媒粒子の量などにもよるが、エチレンなどの有機ガス濃度を0.1ppm以下に低減させることができる。
本実施形態の酸化触媒層33は、基材31の表面に形成される。具体的には、フィルター状やメッシュ状など通気可能な形状を有する基材31の通気部分35に面する表面にその通気性が保たれる状態で(具体的には基材の通気部分35の通気性が維持される状態で)膜状に形成される。基材31は、気体が透過できる構造の部材ならば、板状、シート状あるいは多孔質なブロック体でも構わない。多孔質なブロック体として、ハニカム状の空隙を有する部材は表面積が広く通気性の良好な形態であり当該基材として好ましい。
メソ孔37の形状やその開口部の位置関係などは特に限定されず、例えば膜状支持体34の上面と下面が直線状に連通したシリンダー形状でも、メソ孔が支持体34内部で分岐して他のメソ孔とつながっているようないわゆる連通構造でもよい。連通構造はより多くの開口部がつながっているので、支持体34内部に水分が付着しても通気性が損なわれにくいため、連通構造のほうがより好ましい。
なお、酸化触媒粒子の平均粒径は透過型電子顕微鏡(TEM)の画像写真での個々の粒子サイズを算出し、その平均値として得ることができる。
基材31を用いることで、容易に支持体34の膜状の形状を維持することができる。
さらに、基材31には、ポリイミド、ポリエーテルエーテルケトン、ポリフェニレンスルフィド、ポリアラミド、ポリベンゾチアゾール、ポリベンゾオキサゾール、ポリベンゾイミダゾール、ポリキノリン、ポリキノキサリン、フッ素樹脂などや、フェノール樹脂やエポキシ樹脂などの熱硬化性樹脂などの当業者に公知な耐熱性有機高分子材料を用いることも可能である。
メソ孔37を有する膜状の支持体34は、例えば、支持体内部のメソ孔の鋳型として作用する物質が含有している状態で基材31上に膜状の前駆体を形成し、その後鋳型として作用する物質を分解除去することで得ることができる。
この前駆体溶液を基材31に塗布し、加熱することで溶媒を揮散させるとともに、シラノール基もしくは金属水酸化物を縮合硬化させて、基材31表面に膜状支持体の前駆体を形成させる。その後、さらに300℃以上の高温に焼成することで、前駆体中の鋳型である界面活性剤を分解揮発させることにより除去し、メソ孔を有する膜状支持体34が得られる。
なお、界面活性剤やアルコキシシランもしくは金属アルコキシドの割合は特に限定されず、適宜設定できる。界面活性剤/アルコキシシランもしくは金属アルコキシドのモル比を変えることで、得られる膜状支持体34の細孔体積率、多孔度を制御することができる。
まず、膜状支持体34と担持させる酸化触媒粒子に対応する白金化合物および/またはパラジウム化合物が溶解している溶液(以下、金属化合物溶液と称する)とを接触させて膜状支持体のメソ孔に金属化合物溶液を導入する。その後、焼成および/または還元処理を行いメソ孔内に酸化触媒粒子を形成することにより、本実施形態の酸化触媒層33を得ることができる。
より具体的には、金属化合物溶液を20~90℃、好ましくは50~70℃に加温、攪拌しながら、pH3~10、好ましくはpH5~8になるようにアルカリ溶液を用いて調整する。その後、その表面に膜状支持体34が形成されている基材31を金属化合物溶液に浸漬し、続いて、減圧脱気処理を行い細孔に金属化合物溶液を浸透させた後、200~600℃の加熱焼成処理を行うことで細孔内に白金酸化物および/またはパラジウム酸化物を含む粒子を得ることができる。
白金化合物および/またはパラジウム化合物溶液における白金化合物および/またはパラジウム化合物の濃度は特に限定されないが、1×10-2~1×10-5mol/Lとして溶液を調製するのが、生成した酸化触媒粒子が凝集しにくいので好ましい。
本実施形態に係る送風機構10は、被処理気体を酸化触媒層33に送風することで酸化触媒層33に被処理気体を強制的に接触させる(図1)。これにより、当該気体中に含まれる有機ガス濃度をより効率的に低減させることができる。よって送風機構10は触媒層33の触媒が酸化反応処理できる量の風量を送達できればよく、必要な風量は装置の能力設計に基づいて設計すればよいが、送風の空間速度が10,000/h以上150,000/h以下とするのが望ましい。
送風の空間速度が10,000/h未満であると酸化触媒層33に送達される被処理気体量が少なく、有機ガスの酸化除去量も少なくなるため、範囲内にある場合と比較して当該装置を設置した環境の有機ガス濃度の低減量が小さい。また150,000/hより大きい空間速度であると触媒の酸化除去率が低下するので、被処理気体中の有機ガス濃度の低下が小さく、やはり、範囲内にある場合と比較して当該装置を設置した環境の有機ガス濃度の低減量が小さくなる。
なお上述の空間速度とは、触媒層を通過した被処理気体の単位時間当たりの体積を当該触媒層の体積で除したものと定義する。
また、送風機構10等によって生じた気流が触媒層33及び後述の抗菌等剤を備える部材以外の機能層と接触するように送風機構10を配置してもよい。例えば、機能層として、空気中の埃など浮遊物を除去する防塵フィルターを酸化触媒層33より空気流通方向上流側に設置してもよい。防塵フィルターを設置することで、空気中の浮遊物が酸化触媒層33に付着して被処理気体と酸化触媒層33の接触を阻害して有機ガスの分解が進まないことの防止に寄与することができる。
抗菌性および抗ウイルス性の少なくとも一つを有する化合物(以下、抗菌抗ウイルス剤と呼ぶ)は、例えば、ポリフェノール化合物、第4級アンモニウム塩、無機銅化合物、無機銀化合物、亜鉛、鉄などの原子を含む無機化合物、銅、銀、亜鉛、鉄などの原子を含む有機化合物、白金、ヨウ素化合物、ピリジン系化合物、エステル系化合物、スルファミド系化合物などがある。
これらの抗菌等剤は、2種以上を組み合わせて含有させてもよい。
例のみに限定されるものではない。
ビーカーにテトラエトキシシラン(TEOS)10.4gを入れ、さらにエタノール12.0gを加えた。ここに、さらに0.01M塩酸4.5gを加え、室温で20分攪拌した(A液)。別のビーカーに非イオン系界面活性剤(Brij56)3.3g及びエタノール8.0gを加え、室温で30分攪拌した(B液)。その後、A液にB液を加え、室温条件下で混合し、さらに3時間攪拌し、メソポーラスシリカの前駆体溶液を得た。メソポーラスシリカ前駆体溶液に、基材となるセラミックハニカム(岩谷産業社製)を浸漬させ、15分間減圧した。その後、セラミックハニカムを引上げ余剰分の溶液をエアブローで除去した後、1℃/分で昇温し、450℃で4時間焼成しメソポーラスシリカ膜を固定化したセラミックハニカム基材を得た。
その後、メソポーラスシリカ膜を固定化したセラミックハニカムにジアンミンジニトロ白金硝酸を含む溶液に浸漬させ、余剰分の溶液をエアブローで除去し、水素ガス10%、窒素ガス90%の還元処理ガス中で250℃、1時間焼成し、白金の酸化触媒層を有するハニカム基材を得た。
なおメソポーラスシリカ膜(Pt粒子を含む、以下同じ)に対するPtの担持量は1wt%であった。細孔径をBET法による測定を実施したところ、3.2nmであった。また、メソポーラスシリカ膜の膜厚は500nmであった。また、Ptの粒子サイズをTEMで観察したところ、2.8nmであった。
得られたハニカム基材の酸化触媒層に被処理気体が透過するように送風機構(膜厚方向と直行する方向に被処理気体を送風、比較例1も同じ)を取り付け、有機ガス低減装置を作製した。
ビーカーに酸化チタンコーティング剤(石原産業製ST-K211)を入れ、さらにセラミックハニカム(岩谷産業社製)を浸漬させ、15分間減圧した。その後、セラミックハニカムを引上げ余剰分の溶液をエアブローで除去した後、1℃/分で昇温し、450℃で4時間焼成し酸化チタンをコーティングしたセラミックハニカムを得た。
得られたハニカム基材の酸化触媒層に被処理気体が透過するように送風機構を取り付け、有機ガス低減装置を作製した。
容積120Lの密閉空間内を温度5℃、湿度90%およびエチレン濃度が0.5ppmになるように調整した。その後、密閉空間内に実施例1の有機ガス低減装置を設置し、酸化触媒層を有するハニカム基材に対し空間速度48,000/hで送風しながら、密閉空間内のエチレンの濃度変化を経時的に測定した。なお、空間速度は酸化触媒層の体積300cm3(10cm×10cm×3cm)に対し、風量14.4m3/hから算出した。
酸化触媒層を有するハニカム基材に対し空間速度96,000/hで送風した以外は試験例11と同様の方法で実施した。 なお、空間速度は酸化触媒層の体積300cm3(10cm×10cm×3cm)に対し、風量28.8m3/hから算出した。
有機ガス低減装置を設置しなかったこと以外は試験例1と同様の方法で実施し、その密閉空間内のエチレンの濃度変化を経時的に測定した。
酸化触媒層を有するハニカム基材に対し空間速度300,000/hで送風した以外は試験例1と同様の方法で実施した。なお、空間速度は酸化触媒層の体積300cm3(10cm×10cm×3cm)に対し、風量90m3/hから算出した。
比較例1の有機ガス低減装置を設置し、紫外線ランプを備えたユニットを用いて紫外線照度10W/m2の紫外線を照射し、空間速度48,000/hで送風した以外は試験例4と同様の方法で実施した。なお、空間速度は酸化チタンをコーティングしたセラミックハニカムの体積300cm3(10cm×10cm×3cm)に対し、風量14.4m3/hから算出した。
11 電動ファン
30 酸化触媒層を有する部材
31 基材
33 酸化触媒層
34 膜状支持体
35 通気部分
37 メソ孔
50 抗菌等剤を有する部材
100 有機ガス低減装置
Claims (7)
- 通気性を有し、その表面にメソ孔を有する膜状支持体が形成されている部材と、前記膜状支持体に160℃未満の被処理気体(内燃機関から発生する排気ガスを除く)を供給する気体供給部とを備え、
前記膜状支持体のメソ孔において白金、パラジウムの単体およびこれらの酸化物からなる群から1種または2種以上選択される物質を含む酸化触媒粒子が担持されており、
前記膜状支持体の膜厚が50nm以上500nm以下であり、
前記気体供給部が被処理気体を膜状支持体に送風する送風機構をさらに備え、前記送風機構による送風の空間速度が10,000/h以上150,000/h以下であり、
前記膜状支持体に供給された被処理気体中の有機ガスを酸化することを特徴とする有機ガス低減装置。 - 前記被処理気体中に含まれる有機ガスがエチレンであることを特徴とする請求項1に記載の有機ガス低減装置。
- 前記部材のさらに空気流通方向上流側に配置される抗菌性、防カビ性、抗ウイルス性のうち少なくとも一つを有する化合物を担持する部材をさらに備えることを特徴とする請求項1または2に記載の有機ガス低減装置。
- 前記膜状支持体がSiO2で形成されていることを特徴とする請求項1から3のいずれか一つに記載の有機ガス低減装置。
- 前記メソ孔のBET法で測定した平均孔径が2nm以上10nm以下であることを特徴とする請求項1から4のいずれか一つに記載の有機ガス低減装置。
- 前記酸化触媒粒子の平均粒径が1nm以上10nm以下であることを特徴とする請求項1から5のいずれか一つに記載の有機ガス低減装置。
- メソ孔を有し、当該メソ孔内に白金、パラジウムの単体およびこれらの酸化物からなる群から1種または2種以上選択される物質を含む酸化触媒粒子を担持しており、その膜厚が50nm以上500nm以下である膜状支持体に対し、空間速度10,000/h以上150,000/h以下で送風を行うことにより160℃未満の被処理気体(内燃機関から発生する排気ガスを除く)を供給して拡散させ、当該気体に含有される有機ガス濃度を低減させることを特徴とする有機ガス低減方法。
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