Yun Jiang , Lei Gao , Jianyong Dai , Caiting Li , Huiyu Xiong , Yeling Li , Zhichao Liu , Wenjun Wang , Junhao Hu
{"title":"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","authors":"Yun Jiang , Lei Gao , Jianyong Dai , Caiting Li , Huiyu Xiong , Yeling Li , Zhichao Liu , Wenjun Wang , Junhao Hu","doi":"10.1016/j.jes.2024.04.029","DOIUrl":null,"url":null,"abstract":"<div><p>A chain of GdCe oxides boosted biochars derived from maize straw and sewage sludge (Gd<sub>y</sub>Ce<sub>1-y</sub>/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 H<sub>2</sub>-TPR. Meanwhile, 10%Gd<sub>0.25</sub>Ce<sub>0.75</sub>/MPB exhibited excellent performance, favorable SO<sub>2</sub> 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 O<sub>2</sub>, SO<sub>2</sub>, H<sub>2</sub>O on HCHO abatement over 10 %Gd<sub>0.25</sub>Ce<sub>0.75</sub>/MPB were tested, and the findings demonstrated that the suppressive effects of SO<sub>2</sub> and H<sub>2</sub>O outweighed the promoting influence of O<sub>2</sub> 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 GdO<sub>x</sub> and CeO<sub>x</sub> 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 CeO<sub>x</sub>. According to in situ DRIFTS, a series of intermediates including formate species and dioxymethylene (DOM) were produced, which would eventually decompose into H<sub>2</sub>O and CO<sub>2</sub>. 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%Gd<sub>0.25</sub>Ce<sub>0.75</sub>/MPB possessed remarkable potential for industrial applications.</p></div>","PeriodicalId":15788,"journal":{"name":"Journal of Environmental Sciences-china","volume":null,"pages":null},"PeriodicalIF":5.9000,"publicationDate":"2024-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Unravelling the synergistic effects in GdCe composite oxides supported biochar catalysts for formaldehyde elimination: Elevated performance and SO2 toleration\",\"authors\":\"Yun Jiang , Lei Gao , Jianyong Dai , Caiting Li , Huiyu Xiong , Yeling Li , Zhichao Liu , Wenjun Wang , Junhao Hu\",\"doi\":\"10.1016/j.jes.2024.04.029\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>A chain of GdCe oxides boosted biochars derived from maize straw and sewage sludge (Gd<sub>y</sub>Ce<sub>1-y</sub>/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 H<sub>2</sub>-TPR. Meanwhile, 10%Gd<sub>0.25</sub>Ce<sub>0.75</sub>/MPB exhibited excellent performance, favorable SO<sub>2</sub> 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 O<sub>2</sub>, SO<sub>2</sub>, H<sub>2</sub>O on HCHO abatement over 10 %Gd<sub>0.25</sub>Ce<sub>0.75</sub>/MPB were tested, and the findings demonstrated that the suppressive effects of SO<sub>2</sub> and H<sub>2</sub>O outweighed the promoting influence of O<sub>2</sub> 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 GdO<sub>x</sub> and CeO<sub>x</sub> 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 CeO<sub>x</sub>. According to in situ DRIFTS, a series of intermediates including formate species and dioxymethylene (DOM) were produced, which would eventually decompose into H<sub>2</sub>O and CO<sub>2</sub>. 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%Gd<sub>0.25</sub>Ce<sub>0.75</sub>/MPB possessed remarkable potential for industrial applications.</p></div>\",\"PeriodicalId\":15788,\"journal\":{\"name\":\"Journal of Environmental Sciences-china\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.9000,\"publicationDate\":\"2024-04-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Environmental Sciences-china\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1001074224002080\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENVIRONMENTAL SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Sciences-china","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1001074224002080","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
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.
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.