田軍吉,楊勝芬，陸　鄒，石　宇

(1.貴州省六盤水市鐘山區(qū)經(jīng)濟(jì)和信息化局,貴州 六盤水 553001;2.信和匯金信息咨詢(北京)有限公司,貴州 六盤水 553001)

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綜述與展望

V-Ti基脫硝催化劑去除汞和PCDDs/PCDFs的研究現(xiàn)狀

田軍吉1*,楊勝芬2，陸鄒1，石宇1

(1.貴州省六盤水市鐘山區(qū)經(jīng)濟(jì)和信息化局,貴州 六盤水 553001;2.信和匯金信息咨詢(北京)有限公司,貴州 六盤水 553001)

摘要：將柔軟纖維與折皺鋼網(wǎng)復(fù)合制成波紋式支撐骨架，將V-Ti基脫硝催化劑負(fù)載到波紋式支撐骨架上制成整體波紋式脫硝催化劑。介紹V-Ti基波紋式整體脫硝催化劑的主要制備工藝、優(yōu)點(diǎn)以及國(guó)內(nèi)外對(duì)V-Ti基波紋式整體脫硝催化劑的研究現(xiàn)狀；對(duì)V-Ti基脫硝催化劑與貴金屬脫硝催化劑的制造成本以及PCDDs/PCDFs催化分解效果進(jìn)行對(duì)比，兩者具有相同的催化分解效果，V-Ti基脫硝催化劑成本低得多；活性組分、V質(zhì)量分?jǐn)?shù)以及活性溫度不同，V-Ti基脫硝催化劑催化分解PCDDs/PCDFs的效果也不同，催化分解率最高可達(dá)97.7%；研究者得出V-Ti基脫硝催化劑催化氧化Hg0的不同效果，介紹V-Ti基脫硝催化劑催化氧化Hg0的研究現(xiàn)狀。

關(guān)鍵詞：三廢處理與綜合利用；V-Ti基脫硝催化劑；波紋式脫硝催化劑；汞；PCDDs/PCDFs

CLC number:TQ426.6;X701Document code: AArticle ID: 1008-1143(2016)05-0025-06

目前，火電廠、高爐轉(zhuǎn)爐煉鐵和煉鋼、水泥行業(yè)燃煤煙氣脫硝處理最有效的手段是SCR噴氨脫硝系統(tǒng)[1-9 ]。SCR噴氨系統(tǒng)核心是脫硝催化劑，工業(yè)常用的脫硝催化劑為V-Ti基催化劑，其催化反應(yīng)活性溫度窗口寬，為(300～420)℃。脫硝催化劑使用較多的是蜂窩式和波紋式，波紋式脫硝催化劑具有接觸面積和壓降大的特點(diǎn)，備受燃煤工廠青睞。研究發(fā)現(xiàn)，V-Ti基催化劑不僅可用于煙氣脫硝處理，還可將煙氣中PCDDs/PCDFs催化氧化分解為H2O、CO2和HCl[10-11]，將Hg0催化氧化為Hg2+[12]。

本文綜述波紋式脫硝催化劑的制備工藝、主要特點(diǎn)以及脫硝催化劑催化分解PCDDs/PCDFs和催化氧化汞的主要特性。

1波紋式脫硝催化劑的特點(diǎn)及制備工藝

波紋式脫硝催化劑屬非均質(zhì)催化劑，以柔軟纖維和折皺鋼網(wǎng)復(fù)合制成載體，將活性組分V2O5和V2O5-WO3等涂覆在載體上而制成。波紋式脫硝催化劑以玻璃纖維、陶瓷纖維或復(fù)合式載體作為支撐骨架，結(jié)構(gòu)堅(jiān)硬，承載能力強(qiáng)，還具有以下特點(diǎn)[13]：(1) 主要采用玻璃纖維作為基體材料，與傳統(tǒng)的蜂窩式和板式脫硝催化劑相比，在制造工藝和結(jié)構(gòu)上，融合了兩種催化劑的優(yōu)點(diǎn)；(2) 具有較大的比表面積，脫硝率高于90%，同體積條件下，催化效率優(yōu)于其他脫硝催化劑；(3) 相同的催化效率，波紋式催化劑使用的活性原料少，每立方米質(zhì)量比蜂窩式輕(50～100) kg，以100 m3計(jì)算，催化劑原料使用量降低(5～10) t；(4) 制備工藝相對(duì)簡(jiǎn)單，生產(chǎn)自動(dòng)化程度高。

自20世紀(jì)60年代末開始，日本的三菱、武田化工和日立三家公司研制出以TiO2為基材的催化劑，并逐漸取代Pt-Rh和Pt系列催化劑。該類催化劑主要由V2O5(WO3)、Fe2O3、CrOx、CuO、MnOx、MoO3、NiO和MgO等金屬氧化物或有聯(lián)合作用的混和物構(gòu)成，通常以TiO2、ZrO2、Al2O3、SiO2和AC等作為載體，與SCR系統(tǒng)中的液氨或CO(NH2)2等還原劑發(fā)生還原反應(yīng)，成為電廠SCR脫硝工程中應(yīng)用較廣泛的主流催化劑產(chǎn)品。

國(guó)內(nèi)主流SCR脫硝催化劑核心技術(shù)為美國(guó)、日本、韓國(guó)、丹麥和德國(guó)等國(guó)家壟斷，技術(shù)壁壘高，我國(guó)主要靠高成本引進(jìn)技術(shù)進(jìn)行生產(chǎn)經(jīng)營(yíng)。大榮環(huán)保科技有限公司引進(jìn)韓國(guó)先進(jìn)技術(shù),建成國(guó)內(nèi)首個(gè)9 000 m3·a-1波紋式脫硝催化劑項(xiàng)目，現(xiàn)已在西安經(jīng)濟(jì)開發(fā)區(qū)啟源裝備園區(qū)投產(chǎn)。

2脫硝催化劑催化分解PCDDs/PCDFs

PCDDs/PCDFs化學(xué)性質(zhì)相對(duì)穩(wěn)定，對(duì)生物具有很大的毒害性，因此，如何去除PCDDs/PCDFs的研究受到重視。能催化分解PCDDs/PCDFs的催化劑有貴金屬催化劑和過渡金屬催化劑，雖然貴金屬催化劑催化分解PCDDs/PCDFs的效率最高可達(dá)90%，但貴金屬資源稀缺，價(jià)格昂貴，在批量生產(chǎn)和應(yīng)用中受到限制；以過渡金屬作為催化劑活性組分的主要有VOx、MnOx、CrOx和FeOx等，其中，VOx催化活性最高，V2O5/TiO2催化劑分解PCDDs/PCDFs的效果最好[14]。V2O5-WO3/TiO2催化劑可同時(shí)用于催化還原NOx和催化分解PCDDs/PCDFs[15]。

3脫硝催化劑催化氧化汞的性能

燃煤產(chǎn)生的汞約占人為釋放量的30%，在燃煤煙氣中，汞通常以單質(zhì)汞Hg0、氣態(tài)二價(jià)汞Hg2+及固態(tài)顆粒汞Hgp形式存在，其中，Hg0約占煙氣中汞含量的70%[25]。Hg2+與固態(tài)顆粒汞Hgp可通過濕法脫硫、煙氣除塵和MCFB煙氣凈化系統(tǒng)去除[26-27]。但Hg0易揮發(fā)且不溶于水，可通過吸附劑除去煙氣中的Hg0[28-32]。通過對(duì)煤采用沉重分離、程序升溫?zé)峤?、酸性提取和SSE技術(shù)等研究無煙煤、褐煤和瀝青煤釋放汞的溫度條件以及吸收方法進(jìn)行預(yù)處理[33]，研究[34-36]發(fā)現(xiàn)，在溫度低于150℃、(150～250)℃、(250～400)℃和(400～600)℃時(shí)，汞分別以單質(zhì)汞Hg0、HgCl2、HgS和硫鐵礦鍵配位Hg形式釋放，HNO3提取法對(duì)除去硫鐵鍵配位汞具有較好的效果。工業(yè)用V-Ti基脫硝催化劑通過催化氧化能夠有效地將Hg0氧化成Hg2+[37-38 ]。

4結(jié)語(yǔ)與展望

雖然V系脫硝催化劑在催化氧化汞和催化分解PCDDs/PCDFs方面已有研究，但V-Ti基催化劑催化氧化Hg0和催化分解PCDDs/PCDFs的條件與催化還原NOx的條件存在差異，一是活性溫度不同，催化氧化Hg0的最佳活性溫度為(300～350)℃，催化分解PCDDs/PCDFs的最佳活性溫度為(200～300)℃，而催化還原NOx的最佳活性溫度為(300～420)℃；二是修飾劑的影響，在V-Ti基催化劑中加入修飾成分WO3(MoO3)后有利于促進(jìn)Hg0和NOx的催化氧化還原反應(yīng)，但對(duì)PCDDs/PCDFs的催化分解有抑制作用。研究V-Ti基催化劑催化分解PCDDs/PCDFs時(shí)，PCDDs/PCDFs主要是采用多氯苯和芳香烴混合而成的模擬氣體進(jìn)行研究，所得實(shí)驗(yàn)結(jié)果可能存在一定偏差。針對(duì)V-Ti基催化劑應(yīng)用技術(shù)研究還有待進(jìn)一步深入：

(1) 深入對(duì)V-Ti基催化劑成型工藝研究。雖然在國(guó)外波紋式V-Ti基脫硝催化劑技術(shù)已成熟，但由于國(guó)內(nèi)煙氣成分和相應(yīng)成分含量不同，因此，研究適合國(guó)內(nèi)生產(chǎn)的波紋式V-Ti基脫硝催化劑應(yīng)用技術(shù)或催化劑成型產(chǎn)品迫在眉睫。

(2) 深入對(duì)V-Ti基催化劑催化氧化Hg0和催化分解PCDDs/PCDFs的機(jī)理及影響因素研究。研究加入不同修飾劑修飾V-Ti基催化劑催化氧化Hg0的機(jī)理影響，進(jìn)一步提高V-Ti基催化劑催化氧化Hg0的效率；研究催化分解真正的PCDDs/PCDFs，真正了解催化分解PCDDs/PCDFs的機(jī)理和影響因素。

(3) 深入對(duì)工業(yè)用V-Ti催化劑改性研究。加深對(duì)現(xiàn)有V-Ti基催化劑改性研究，使改性后的V2O5-WO3(MoO3)/TiO2催化劑在最佳脫硝條件下能同時(shí)得到催化氧化Hg0和催化分解PCDDs/PCDFs的效率。

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Research status of V-Ti-based denitrification catalysts for removal of Hg and PCDDs/PCDFs

Tian Junji1*, Yang Shengfen2, Lu Zou1, Shi Yu1

(1.Economic and Information Bureau of Zhong Mountain Area of Liupanshui City, Liupanshui 553001,Guizhou, China; 2.Xinhe Huijin Consulting (Beijing) Co. Ltd, Liupanshui 553001, Guizhou, China)

Abstract:The composite corrugated support frames were prepared by using the soft fibers and creasing steel mesh.The monolithic corrugated denitrification catalysts were prepared by loading V-Ti-based De-NOx catalysts onto corrugated support frames.The current major preparation processes,main advantages and research status of V-Ti-based corrugated denitrification catalysts at home and abroad were reviewed.Compared V-Ti-based denitrification catalysts with noble metal denitrification catalysts,both catalysts possessed the same catalytic decomposition effects of PCDDs/PCDFs,but the manufacturing cost of V-Ti-based denitrification catalysts was lower than those of noble metal denitrification catalysts.V-Ti-based denitrification catalysts with different active components,vanadium contents and reaction activity temperatures exhibited different catalytic decomposition effects of PCDDs/PCDFs.The highest catalytic decomposition rate was 97.7%.The researchers obtained different catalytic effects of V-Ti-based denitrification catalysts for oxidation of Hg0.The research status of V-Ti-based denitrification catalyst for catalytic oxidation of Hg0 oxidation was introduced.

Key words:three waste disposal and comprehensive utilization; V-Ti based denitrification catalyst; corrugated denitrification catalyst; Hg; PCDDs/PCDFs

收稿日期：2015-11-12；修回日期：2016-04-12

作者簡(jiǎn)介：田軍吉，1987年生，男，貴州省銅仁市人，主要從事新型環(huán)保材料、工業(yè)煙氣排放后處理技術(shù)和柴油煙氣催化凈化研究。

doi:10.3969/j.issn.1008-1143.2016.05.005 10.3969/j.issn.1008-1143.2016.05.005

中圖分類號(hào)：TQ426.6;X701

文獻(xiàn)標(biāo)識(shí)碼：A

文章編號(hào)：1008-1143(2016)05-0025-06

通訊聯(lián)系人：田軍吉。