揭示 GdCe 复合氧化物支撑生物炭催化剂消除甲醛的协同效应:提高性能和二氧化硫耐受性

IF 5.9 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Journal of Environmental Sciences-china Pub Date : 2024-04-30 DOI:10.1016/j.jes.2024.04.029
Yun Jiang , Lei Gao , Jianyong Dai , Caiting Li , Huiyu Xiong , Yeling Li , Zhichao Liu , Wenjun Wang , Junhao Hu
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引用次数: 0

摘要

利用玉米秸秆和污水污泥制备了一系列钆铈氧化物助生物炭(GdyCe1-y/MPBs),用于催化分解甲醛(HCHO)。通过 XPS、原位 DRIFTS、BET、XRD、SEM 和 H2-TPR 等方法全面评估了甲醛分解性能与相应结构特征之间的内在联系。同时,10%Gd0.25Ce0.75/MPB 表现出优异的性能,在 160 至 320 ℃ 的宽温度范围内具有良好的二氧化硫和湿气耐受性,在 200 ℃ 时的脱除效率达到 96.8%,选择性为 90.5%。测试了 O2、SO2 和 H2O 对 10 %Gd0.25Ce0.75/MPB 上 HCHO 降解的单一或联合影响,结果表明在特定范围内,SO2 和 H2O 的抑制作用大于 O2 的促进作用。与钆或铈单独改性的 MPB 相比,钆和铈共改性的 MPB 具有更优越的 HCHO 去除能力,这归因于 GdOx 和 CeOx 的协同效应,并得益于表面积和总孔体积的增加、表面活性氧物种的增加、氧化还原能力的提高以及 CeOx 结晶的抑制。根据原位 DRIFTS,产生了一系列中间产物,包括甲酸盐类和二氧亚甲基(DOM),这些中间产物最终会分解成 H2O 和 CO2。此外,支撑物的分层多孔结构扩大了反应物的传质和扩散以及催化位点的可达性,这也是其催化性能优异的原因。此外,10%Gd0.25Ce0.75/MPB 具有显著的工业应用潜力。
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Unravelling the synergistic effects in GdCe composite oxides supported biochar catalysts for formaldehyde elimination: Elevated performance and SO2 toleration

A chain of GdCe oxides boosted biochars derived from maize straw and sewage sludge (GdyCe1-y/MPBs) were fabricated for formaldehyde (HCHO) catalytic decomposition. The ingenerate relationship between the abatement performance and corresponding structural feature was comprehensively evaluated by XPS, in situ DRIFTS, BET, XRD, SEM and H2-TPR. Meanwhile, 10%Gd0.25Ce0.75/MPB exhibited excellent performance, favorable SO2 and moisture toleration over a broad temperature range from 160 to 320 ℃, where it achieved 96.8% removal efficiency with 90.5 % selectivity at 200 ℃. The single or united effects of O2, SO2, H2O on HCHO abatement over 10 %Gd0.25Ce0.75/MPB were tested, and the findings demonstrated that the suppressive effects of SO2 and H2O outweighed the promoting influence of O2 within a specific range. Gd and Ce co-modified MPB revealed superior HCHO removal capability in contrast to that of Gd or Ce severally modified MPB, ascribing to the synergistic effect of GdOx and CeOx and benefitting from the augmentation of surface area and total pore volume, the aggrandizement of surface active oxygen species, the promotion of redox ability and the inhibition crystallization of CeOx. According to in situ DRIFTS, a series of intermediates including formate species and dioxymethylene (DOM) were produced, which would eventually decompose into H2O and CO2. In addition, the mass transfer and diffusion of the reactants along with the accessibility of the catalytic sites were enlarged by the hierarchical porous structure of the support, which were also answerable for its distinguished catalytic performance. Furthermore, 10%Gd0.25Ce0.75/MPB possessed remarkable potential for industrial applications.

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来源期刊
Journal of Environmental Sciences-china
Journal of Environmental Sciences-china 环境科学-环境科学
CiteScore
13.70
自引率
0.00%
发文量
6354
审稿时长
2.6 months
期刊介绍: The Journal of Environmental Sciences is an international journal started in 1989. The journal is devoted to publish original, peer-reviewed research papers on main aspects of environmental sciences, such as environmental chemistry, environmental biology, ecology, geosciences and environmental physics. Appropriate subjects include basic and applied research on atmospheric, terrestrial and aquatic environments, pollution control and abatement technology, conservation of natural resources, environmental health and toxicology. Announcements of international environmental science meetings and other recent information are also included.
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