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精選成果簡報(bào) Appl. Catal. B:多孔石墨化炭負(fù)載FeOCl作為雙功能吸附催化劑用于含氯揮發(fā)性有機(jī)化合物的濕式過氧化物氧化:介孔的影響和機(jī)理研究 Porous graphitized carbon-supported FeOCl as a bifunctional adsorbent-catalyst for the wet peroxide oxidation of chlorinated volatile organic compounds: Effect of mesopores and mechanistic study ——武漢大學(xué) 李進(jìn)軍老師課題組 濕式洗滌與吸附增強(qiáng)型異質(zhì)高級(jí)氧化工藝(AOPs)相結(jié)合,是處理含氯揮發(fā)性有機(jī)化合物(CVOCs)的有效方法。武漢大學(xué)李進(jìn)軍老師課題組開發(fā)了一種多孔石墨化炭 (PGC) 負(fù)載的FeOCl催化劑,可有效去除氣態(tài)二氯乙烷、三氯乙烯、二氯甲烷和氯苯。通過BET表征及吸附性能分析得到PGC負(fù)載FeOCl催化劑具有發(fā)達(dá)的介孔結(jié)構(gòu),可加快有機(jī)分子在顆粒內(nèi)的擴(kuò)散,表現(xiàn)出對(duì)CVOCs更好的去除性能。 Chem. Eng. J:微介孔石墨化炭纖維作為疏水吸附劑可去除空氣中的揮發(fā)性有機(jī)化合物 Micro-mesoporous graphitized carbon fiber as hydrophobic adsorbent that removes volatile organic compounds from air 活性炭纖維(ACFs)是一類受歡迎的揮發(fā)性有機(jī)化合物(VOCs)吸附劑,武漢大學(xué)李進(jìn)軍老師課題組采用KOH催化石墨化的方法制備了疏水性增強(qiáng)的多孔石墨化炭纖維(PGCFs),并研究了其對(duì)代表性揮發(fā)性有機(jī)化合物的吸附能力,通過表征表明PGCF具有超過2200 m2/g的高比表面積和微介孔結(jié)構(gòu),在潮濕條件下對(duì)有機(jī)物的選擇性吸附能力得到提高。 Chem. Eng. J:用于吸附揮發(fā)性有機(jī)化合物的竹制疏水多孔石墨化炭 Bamboo-derived hydrophobic porous graphitized carbon for adsorption of volatile organic compounds 采用復(fù)合催化石墨化法制備了疏水竹基多孔石墨化炭(BPGCs),研究其對(duì)甲苯、環(huán)己烷和乙醇的吸附性能,并通過BET表征測(cè)試了不同合成溫度下制備得到的炭材料的比表面積大小、微介孔比例,為評(píng)價(jià)炭材料的吸附性能提供一定的理論支撐。 材料吸附性能表征技術(shù) 通過光催化驅(qū)動(dòng)CO2減排,再加上光氧化轉(zhuǎn)化塑料廢物為增值化學(xué)品,是一種解決溫室和環(huán)境危機(jī)的有效策略。通過比表面及孔徑分析儀對(duì)不同比例下合成的多孔石墨化炭(PGCs)和PGC負(fù)載FeOCl催化劑(FeOCl/PGCs)進(jìn)行表征,N2吸脫附等溫線如下圖1d所示。PGC0和FeOCl/PGC0對(duì)N2的吸附量主要在P/P0< 0.1的低相對(duì)壓力段,這是微孔材料的典型特征。 相比之下,其他PGCs和FeOCl/PGCs的N2吸附量隨相對(duì)壓力的增加而持續(xù)增加,且等溫線均存在滯后環(huán),表明材料中存在介孔結(jié)構(gòu)。FeOCl/PGC催化劑的等溫線特征與其相應(yīng)的PGC載體非常相似,僅存在氮吸收量略有下降的區(qū)別,這表明催化劑負(fù)載并未顯著改變碳材料的孔隙率。由下圖1e的NLDFT孔徑分布和表1的詳細(xì)數(shù)據(jù)可知,石墨化后材料介孔占比增加,炭材料的比表面積隨著石墨化程度的增加而逐漸減小。PGC0、PGC1、PGC3、PGC4和PGC8的對(duì)DCE的去除率分別為26.5%、25.0%、22.2%、19.7%和16.5%。DCE去除效率的順序與PGCs比表面積的順序一致,這歸因于在吸附法濕法洗滌DCE時(shí),隨著吸附位點(diǎn)的逐漸占用,比表面積越大的材料可用的吸附位點(diǎn)越多,去除效果越好。 表征得到的不同炭材料的N2吸脫附等溫線及NLDFT孔徑分布數(shù)據(jù),粘膠基活性炭纖維(VACF)呈現(xiàn)出 I 型等溫線,其在 P/P0< 0.05 的低相對(duì)壓力段氮吸附量急劇增加,而在 P/P0較高時(shí)等溫線趨于平緩,這表明該材料以微孔為主。而多孔石墨化炭纖維(PGCFs)的等溫線除了在低 P/P0段有顯著的氮吸附外,隨著 P/P0的升高,吸附量呈現(xiàn)逐漸增加,表明 PGCF 中同時(shí)存在微孔和介孔。由NLDFT數(shù)據(jù)可知,VACF 的大部分孔寬小于 2 nm,而 PGCF 除了在微孔范圍有分布,在大于 2 nm 的介孔范圍也有集中分布。此外,通過比較材料的比表面積及孔體積詳細(xì)數(shù)據(jù),可以發(fā)現(xiàn)將 VACF 轉(zhuǎn)化為 PGCF 后,比表面積從 1304 m2/g 增加到大于 2200 m2/g,孔體積尤其是介孔體積大幅增加,介孔體積占其總孔隙體積的一半以上。PGCFs比VACF 具有更高的比表面積,進(jìn)一步解釋了 PGCFs 對(duì)甲苯和環(huán)己烷的吸附增強(qiáng)的原因。 對(duì)不同方法制備的生物質(zhì)基活性炭(BACs)和竹基多孔石墨化炭(BPGCs)進(jìn)行比表面及孔徑表征,BAC對(duì)N2的吸附主要發(fā)生在低相對(duì)壓力下(P/P0<0.05),呈現(xiàn)出典型的 I 型等溫線,表明 BAC 以微孔為主。相比之下,BPGCs 除了在 P/P0<0.05 時(shí)有吸附外,隨著 P/P0的增大,氮吸附量仍在增加,并且存在回滯環(huán),表明BPGCs 中同時(shí)存在微孔和中孔。如下表1所示,通過比較不同炭材料的比表面積和孔徑分布詳細(xì)數(shù)據(jù)可知:BAC的介孔體積只占其總孔體積的 20%,而 BPGCs 的介孔體積一般占 44% 以上,其中BPGC-500具有較大的表面積(2181 m2/g)和較高的介孔體積,BPGC的較大的介孔體積可以有助于在吸收乙醇后冷凝水有足夠的空間進(jìn)行體積膨脹。 國儀量子比表面及孔徑分析儀 國儀量子V-Sorb X800系列比表面及孔徑分析儀采用靜態(tài)容量法測(cè)試原理,具備充分的自動(dòng)化操作,人性化的操作界面,簡單易學(xué),廣泛應(yīng)用于催化材料、環(huán)保材料、電池材料及納米材料等領(lǐng)域。產(chǎn)品技術(shù)通過機(jī)械工業(yè)聯(lián)合會(huì)科技成果鑒定,被歐美高校、科研實(shí)驗(yàn)室選購使用,獲得,樹立了優(yōu)良的國產(chǎn)品牌形象。 助力成果目錄 1.Porous graphitized carbon-supported FeOCl as a bifunctional adsorbent-catalyst for the wet peroxide oxidation of chlorinated volatile organic compounds: Effect of mesopores and mechanistic study. Applied Catalysis B: Environmental(2023)2.Micro-mesoporous graphitized carbon fiber as hydrophobic adsorbent that removes volatile organic compounds from air. Chemical Engineering Journal(2023)3.Bamboo-derived hydrophobic porous graphitized carbon for adsorption of volatile organic compounds. Chemical Engineering Journal(2023)4.Chiral Nanosilica Drug Delivery Systems Stereoselectively Interacted with the Intestinal Mucosa to Improve the Oral Adsorption of Insoluble Drugs. ACS Nano(2023)5.A facile“thick to thin"strategy for integrating high volumetric energy density and excellent flexibility into MXene/wood free-standing electrode for supercapacitors. Chemical Engineering Journal(2023)6.The efficiency and mechanism of excess sludge-based biochar catalyst in catalytic ozonation of landfill leachate. Journal of Hazardous Materials(2023)7.Aqueous Zn-ion batteries using amorphous Zn-buserite with high activity and stability. 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Royal Society of Chemistry(2022)20.Role and significance of water and acid washing on biochar for regulating methane production from waste activated sludge. Science of The Total Environment(2022)21.Soil properties affect vapor-phase adsorption to regulate dimethyl disulfide diffusion in soil. Science of The Total Environment(2022)22.Removal of lead (Pb+2) from contaminated water using a novel MoO3-biochar composite: Performance and mechanism. Environmental Pollution(2022)23.Acid washed lignite char supported bimetallic Ni-Co catalyst for low temperature catalytic reforming of corncob derived volatiles. Energy Conversion and Management(2022)