[1]张志杨,丁子萱,冯迎辰,等.NaZSM-5分子筛提高秸秆水热制备胡敏酸产率的机制[J].江苏农业学报,2024,(11):2083-2092.[doi:doi:10.3969/j.issn.1000-4440.2024.11.012]
　ZHANG Zhiyang,DING Zixuan,FENG Yingchen,et al.Mechanism of NaZSM-5 zeolite in enhancing the yield of humic acid from straws via hydrothermal process[J].,2024,(11):2083-2092.[doi:doi:10.3969/j.issn.1000-4440.2024.11.012]
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NaZSM-5分子筛提高秸秆水热制备胡敏酸产率的机制()
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江苏农业学报[ISSN:1006-6977/CN:61-1281/TN]

卷:
期数:
2024年11期
页码:
2083-2092
栏目:
耕作栽培·资源环境
出版日期:
2024-11-30

文章信息/Info

Title:
Mechanism of NaZSM-5 zeolite in enhancing the yield of humic acid from straws via hydrothermal process
作者:
张志杨1; 2; 3; 丁子萱1; 2; 3; 冯迎辰1; 2; 4; 徐文龙1; 2; 肖清波1; 2; 3; 4
(1.江苏省农业科学院农业资源与环境研究所,江苏南京210014；2.农业农村部盐碱土改良与利用<滨海盐碱地>重点实验室,江苏南京210014；3.江苏大学环境与安全工程学院,江苏镇江212013；4.南京信息工程大学生态与应用气象学院,江苏南京210044)
Author(s):
ZHANG Zhiyang1; 2; 3; DING Zixuan1; 2; 3; FENG Yingchen1; 2; 4; XU Wenlong1; 2; XIAO Qingbo1; 2; 3; 4
(1.Institute of Agricultural Resources and Environment, Jiangsu Academy of Agricultural Sciences, Nanjing 210014, China；2.Key Laboratory of Saline-Alkali Soil Improvement and Utilization (Coastal Saline-Alkali Lands), Ministry of Agriculture and Rural Affairs, Nanjing 210014, China;3.School of Environment and Safety Engineering, Jiangsu University, Zhenjiang 212013, China;4.School of Ecology and Applied Meteorology, Nanjing University of Information Science and Technology, Nanjing 210044, China)
关键词:
NaZSM-5分子筛; 秸秆; 水热; 胡敏酸; 产率
Keywords:
NaZSM-5 molecular sieve; straw; hydrothermal; humic acid; yield
分类号:
TQ44
DOI:
doi:10.3969/j.issn.1000-4440.2024.11.012
文献标志码:
A
摘要:
秸秆水热降解制备腐殖酸是一种重要的秸秆资源化利用途径,但是该过程面临胡敏酸产率较低的问题。本研究拟通过在秸秆水热处理中加入NaZSM-5分子筛,探讨其对胡敏酸产率的影响。结果表明,添加NaZSM-5分子筛能够显著提高胡敏酸的产率,随着NaZSM-5分子筛硅铝比的提高,胡敏酸产率呈现先上升后下降的趋势,其中硅铝比为50的NaZSM-5分子筛能使胡敏酸产率达到16.04%。为了深入探讨NaZSM-5分子筛提高胡敏酸产率的机制,本研究采用X射线光电子能谱、核磁共振波谱、氨气升序升温吸附与脱附、模型化合物季铵盐吸附与脱附、红外光谱等表征技术进行相关分析。结果表明,高硅铝比(200、85)的NaZSM-5分子筛中存在低强度、中强度的Lewis酸性位点；随着硅铝比降低(分别由200、85降至38、25),中强度的Lewis酸性位点逐渐转变为高强度的Lewis酸性位点。在硅铝比为50的NaZSM-5分子筛中,中强度Lewis酸性位点的含量最高,中强度Lewis酸性位点能够有效稳定秸秆水热降解过程中形成的季铵氮结构(R4N),从而促进胡敏酸的生成。高硅铝比的NaZSM-5对季铵氮结构的吸附强度较弱,不利于其转化为胡敏酸,而低硅铝比的NaZSM-5对季铵氮结构的吸附强度较强,可能导致季铵氮结构过度偶联,进而降低胡敏酸产率。本研究结果可为提高秸秆水热降解制备胡敏酸的产率提供一种有效方法,从而进一步推动秸秆的资源化利用。
Abstract:
The hydrothermal preparation of humic acid from straws is a significant method for utilizing straw resources, but it is often hindered by low humic acid yields. This study explored the impact of incorporating NaZSM-5 zeolite into the hydrothermal treatment of straws on humic acid yield. The experimental results indicated that adding NaZSM-5 zeolite significantly enhanced the yield of humic acid. Specifically, as the Si/Al molar ratio of NaZSM-5 increased, the yield of humic acid increased first and then decreased, with a peak yield of 16.04% observed at a Si/Al molar ratio of 50. To elucidate the mechanism of NaZSM-5 zeolite to improve humic acid yield, we employed several characterization techniques, including X-ray photoelectron spectroscopy, nuclear magnetic resonance spectroscopy, NH3 adsorption-desorption, quaternary ammonium salt adsorption-desorption, and infrared spectroscopy. The findings revealed that NaZSM-5 zeolite with high Si/Al molar ratios (200 and 85) contained low to medium strength Lewis acid sites. As the Si/Al molar ratio decreased (from 200 and 85 to 38 and 25), medium-strength Lewis acid sites gradually converted to high-strength Lewis acid sites. The NaZSM-5 zeolite with a Si/Al molar ratio of 50 exhibited the highest content of medium-strength Lewis acid sites. These medium-strength sites effectively stabilized the quaternary ammonium nitrogen structure (R4N) formed during the hydrothermal process, thus facilitating humic acid formation. Conversely, NaZSM-5 with high Si/Al molar ratios showed weaker adsorption strength for the quaternary ammonium nitrogen structure, which hindered its conversion to humic acid. On the other hand, NaZSM-5 with lower Si/Al molar ratios exhibited stronger adsorption, which could lead to excessive coupling of the quaternary ammonium nitrogen structure, thus reducing the yield of humic acid. This study presents an effective method for improving the yield of humic acid through straw hydrothermal treatment, thereby advancing the resource utilization of straws.

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备注/Memo

备注/Memo:
收稿日期：2024-09-04基金项目：国家自然科学基金项目(42407034)；江苏省农业科技自主创新项目[CX(24)3107、CX(20)3079]作者简介：张志杨(1991-),男,安徽合肥人,博士,助理研究员,主要从事新型农业纳米的设计与研究。(E-mail)zhangzy@jaas.ac.cn通讯作者：肖清波,(E-mail)qbxiao@jaas.ac.cn
更新日期/Last Update: 2025-01-20