精选成果简报 Appl. Catal. B:多孔石墨化炭负载FeOCl作为双功能吸附催化剂用于含氯挥发性有机化合物的湿式过氧化物氧化:介孔的影响和机理研究 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 ——武汉大学 李进军老师课题组 湿式洗涤与吸附增强型异质高级氧化工艺(AOPs)相结合,是处理含氯挥发性有机化合物(CVOCs)的有效方法。武汉大学李进军老师课题组开发了一种多孔石墨化炭 (PGC) 负载的FeOCl催化剂,可有效去除气态二氯乙烷、三氯乙烯、二氯甲烷和氯苯。通过BET表征及吸附性能分析得到PGC负载FeOCl催化剂具有发达的介孔结构,可加快有机分子在颗粒内的扩散,表现出对CVOCs更好的去除性能。 Chem. Eng. J:微介孔石墨化炭纤维作为疏水吸附剂可去除空气中的挥发性有机化合物 Micro-mesoporous graphitized carbon fiber as hydrophobic adsorbent that removes volatile organic compounds from air 活性炭纤维(ACFs)是一类受欢迎的挥发性有机化合物(VOCs)吸附剂,武汉大学李进军老师课题组采用KOH催化石墨化的方法制备了疏水性增强的多孔石墨化炭纤维(PGCFs),并研究了其对代表性挥发性有机化合物的吸附能力,通过表征表明PGCF具有超过2200 m2/g的高比表面积和微介孔结构,在潮湿条件下对有机物的选择性吸附能力得到提高。 Chem. Eng. J:用于吸附挥发性有机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 采用复合催化石墨化法制备了疏水竹基多孔石墨化炭(BPGCs),研究其对甲苯、环己烷和乙醇的吸附性能,并通过BET表征测试了不同合成温度下制备得到的炭材料的比表面积大小、微介孔比例,为评价炭材料的吸附性能提供一定的理论支撑。 材料吸附性能表征技术 通过光催化驱动CO2减排,再加上光氧化转化塑料废物为增值化学品,是一种解决温室和环境危机的有效策略。通过比表面及孔径分析仪对不同比例下合成的多孔石墨化炭(PGCs)和PGC负载FeOCl催化剂(FeOCl/PGCs)进行表征,N2吸脱附等温线如下图1d所示。PGC0和FeOCl/PGC0对N2的吸附量主要在P/P0< 0.1的低相对压力段,这是微孔材料的典型特征。 相比之下,其他PGCs和FeOCl/PGCs的N2吸附量随相对压力的增加而持续增加,且等温线均存在滞后环,表明材料中存在介孔结构。FeOCl/PGC催化剂的等温线特征与其相应的PGC载体非常相似,仅存在氮吸收量略有下降的区别,这表明催化剂负载并未显著改变碳材料的孔隙率。由下图1e的NLDFT孔径分布和表1的详细数据可知,石墨化后材料介孔占比增加,炭材料的比表面积随着石墨化程度的增加而逐渐减小。PGC0、PGC1、PGC3、PGC4和PGC8的对DCE的去除率分别为26.5%、25.0%、22.2%、19.7%和16.5%。DCE去除效率的顺序与PGCs比表面积的顺序一致,这归因于在吸附法湿法洗涤DCE时,随着吸附位点的逐渐占用,比表面积越大的材料可用的吸附位点越多,去除效果越好。 表征得到的不同炭材料的N2吸脱附等温线及NLDFT孔径分布数据,粘胶基活性炭纤维(VACF)呈现出 I 型等温线,其在 P/P0< 0.05 的低相对压力段氮吸附量急剧增加,而在 P/P0较高时等温线趋于平缓,这表明该材料以微孔为主。而多孔石墨化炭纤维(PGCFs)的等温线除了在低 P/P0段有显著的氮吸附外,随着 P/P0的升高,吸附量呈现逐渐增加,表明 PGCF 中同时存在微孔和介孔。由NLDFT数据可知,VACF 的大部分孔宽小于 2 nm,而 PGCF 除了在微孔范围有分布,在大于 2 nm 的介孔范围也有集中分布。此外,通过比较材料的比表面积及孔体积详细数据,可以发现将 VACF 转化为 PGCF 后,比表面积从 1304 m2/g 增加到大于 2200 m2/g,孔体积尤其是介孔体积大幅增加,介孔体积占其总孔隙体积的一半以上。PGCFs比VACF 具有更高的比表面积,进一步解释了 PGCFs 对甲苯和环己烷的吸附增强的原因。 对不同方法制备的生物质基活性炭(BACs)和竹基多孔石墨化炭(BPGCs)进行比表面及孔径表征,BAC对N2的吸附主要发生在低相对压力下(P/P0<0.05),呈现出典型的 I 型等温线,表明 BAC 以微孔为主。相比之下,BPGCs 除了在 P/P0<0.05 时有吸附外,随着 P/P0的增大,氮吸附量仍在增加,并且存在回滞环,表明BPGCs 中同时存在微孔和中孔。如下表1所示,通过比较不同炭材料的比表面积和孔径分布详细数据可知:BAC的介孔体积只占其总孔体积的 20%,而 BPGCs 的介孔体积一般占 44% 以上,其中BPGC-500具有较大的表面积(2181 m2/g)和较高的介孔体积,BPGC的较大的介孔体积可以有助于在吸收乙醇后冷凝水有足够的空间进行体积膨胀。 国仪量子比表面及孔径分析仪 国仪量子V-Sorb X800系列比表面及孔径分析仪采用静态容量法测试原理,具备充分的自动化操作,人性化的操作界面,简单易学,广泛应用于催化材料、环保材料、电池材料及纳米材料等领域。产品技术通过机械工业联合会科技成果鉴定,被欧美高校、科研实验室选购使用,获得,树立了优良的国产品牌形象。 助力成果目录 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. Journal of Materials Chemistry A(2023)8.Rapid complete reconfiguration induced actual active species for industrial hydrogen evolution reaction. Nature Communications(2022)9.Catalytic aromatic ring hydrogenation over ruthenium nanoparticles supported on α-Al2O3 at room temperature. Applied Catalysis B: Environmental(2022)10.Engineered neutrophil apoptotic bodies ameliorate myocardial infarction by promoting macrophage efferocytosis and inflammation resolution. Bioactive Materials(2022)11.Role and significance of co-additive of biochar and nano-magnetite on methane production from waste activated sludge: Non-synergistic rather than synergistic effects. Chemical Engineering Journal(2022)12.Micro-mesoporous graphitized carbon fiber as hydrophobic adsorbent that removes volatile organic compounds from air. Chemical Engineering Journal(2022)13.Mercerization of tubular bacterial nanocellulose for control of the size and performance of small-caliber vascular grafts. 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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)