高性能IrO2/CeO2-ZrO2甲烷燃烧催化剂的设计合成及构效关系研究
结题报告
批准号:
21878053
项目类别:
面上项目
资助金额:
62.0 万元
负责人:
詹瑛瑛
依托单位:
学科分类:
B0803.反应工程
结题年份:
2022
批准年份:
2018
项目状态:
已结题
项目参与者:
郑勇、郑笑笑、肖益鸿、辜冬梅、韩倩倩、金凡、何园园、王杨燕
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中文摘要
含有较低浓度甲烷的油田伴生尾气直接排放严重污染环境,利用甲烷催化燃烧技术实现低浓度甲烷的清洁高效利用是最有效手段,其关键是开发出高性能的甲烷燃烧催化剂。本项目针对现行Pt、Pd等贵金属基催化剂水热稳定性和抗硫性能不足的难题,拟利用均质乳化技术和掺杂稳定剂的方法设计制备出高比表面积、高稳定性的CeO2-ZrO2固溶体载体;并以IrO2为活性组分,设计制备出高性能的IrO2/CeO2-ZrO2甲烷燃烧催化剂。利用各种先进的表征手段,揭示均质乳化预处理和稳定剂掺杂对铈锆固溶体前驱物的影响规律,建立铈锆固溶体的热稳定性与氧空位的调变方法,阐明活性组分IrO2与CeO2-ZrO2固溶体之间的协同作用机制,为适应动态环境条件下的低浓度CH4清洁高效利用提供技术源头。
英文摘要
The oil field associated gas contains low-concentration methane, which will cause the environmental pollution if released directly. Among the technologies developed for the clean and effective utilization of low-concentration methane, the catalytic combustion process is considered as the most promising approach, the key is to develop high efficient catalysts. Nowadays, the common used catalysts for this reaction are noble metals such as Pt and Pd. However, these noble metals generally suffer from the low hydrothermal stability and poor sulfur-resisting performance. To solve these problems, we plan to prepare the CeO2-ZrO2 solid solution as supports through the homogeneous emulsion method and the stabilizer doping strategy. The CeO2-ZrO2 solid solution with high surface area and high stability is benefit for the dispersion of active component IrO2, which may endow the resulting IrO2/CeO2-ZrO2 with high performance for the catalytic combustion of methane. With the various advanced characterizations, we aim to reveal the influence rules of the homogeneous emulsion preprocessing and stabilizer doping on the precursor of CeO2-ZrO2 solid solution. Moreover, we will make effort to establish new methods for the control of the thermal stability and oxygen vacancy of CeO2-ZrO2 solid solution. Finally, the synergistic mechanism between the active component IrO2 and the CeO2-ZrO2 solid solution will also be investigated and elucidated. The achieved findings will provide a technical source for the clean and effective utilization of low-concentration methane under dynamic conditions.
项目针对油田伴生尾气等低浓度甲烷治理体系所需,提出了开展高性能Ir基甲烷燃烧催化剂的设计合成。基于载体形貌、表面性质和组成与活性组分IrOx.前驱体的调变策略,开展了研究工作。采用现代物化手段表征,初步阐明了Ir基催化剂的活性组分与载体之间的协同机制,以及催化剂的微观结构与催化活性间的相关性及其甲烷氧化反应的催化机理。制备出不同系列的适应高空速、低空燃比气氛的Ir基催化剂,而且较好地解决了催化剂抗水性问题。Ir/ZrO2-SO42-催化剂在50,000 mL∙h-1∙gcat -1空速下甲烷完全转化温度的T90%为380 ºC;在体系中含10%H2O条件下,450 ºC 甲烷转化率稳定在90%。Ir/TiO2–ZrO2催化剂的性能与之相近,T90%为388 ºC。鉴于Ir价格攀升近5倍,同时着力于非铱基催化剂的研究。项目研究为低浓度甲烷燃烧催化剂的开发奠定了理论基础,并为Ir基、Pd基、Co基尖晶石以及ZrO2等纳米催化材料的合成改性提供具有参考价值的规律和参数。
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专利列表
Synergistic tuning of the phase structure of alumina and ceria-zirconia in supported palladium catalysts for enhanced methane combustion
协同调节负载钯催化剂中氧化铝和氧化铈-氧化锆的相结构以增强甲烷燃烧
DOI:10.1016/j.ijhydene.2021.07.151
发表时间:2021-08
期刊:International Journal of Hydrogen Energy
影响因子:7.2
作者:Jia Lin;Yelin Chen;Jiangli Huang;Guohui Cai;Yihong Xiao;Yingying Zhan;Ying Zheng
通讯作者:Ying Zheng
Catalytic methane oxidation performance over Pd/γ-Al2O3 catalyst optimized by the synergy of phosphorus and MOx (M = La, Ba and Zr)
通过磷和 MOx(M = La、Ba 和 Zr)的协同作用优化 Pd/γ-Al2O3 催化剂的催化甲烷氧化性能
DOI:10.1016/j.fuel.2021.120933
发表时间:2021-09
期刊:Fuel
影响因子:7.4
作者:Xiaohua Chen;Jia Lin;Yong Zheng;Yingying Zhan;Wen Zhang;Yihong Xiao;Ying Zheng;Lilong Jiang
通讯作者:Lilong Jiang
Pd/Al_2O_3 catalysts modified with Mg for catalytic combustion of methane:Effect of Mg/Al mole ratios on the supports and active PdO_x formation
Mg修饰的Pd/Al_2O_3催化剂用于甲烷催化燃烧:Mg/Al摩尔比对载体和活性PdO_x形成的影响
DOI:--
发表时间:2019
期刊:燃料化学学报
影响因子:--
作者:Zhan Yingying;Kang Liang;Zhou Yuchang;Cai Guohui;Chen Chongqi;Jiang Lilong
通讯作者:Jiang Lilong
Rational design of highly H2O- and CO2-tolerant hydroxyapatite-supported Pd catalyst for low-temperature methane combustion
高耐H2O和CO2的羟基磷灰石负载Pd低温甲烷燃烧催化剂的合理设计
DOI:10.1016/j.cej.2020.125225
发表时间:2020-09
期刊:Chemical Engineering Journal
影响因子:15.1
作者:Yangyu Zhang;Jie Zhu;Shusheng Li;Yihong Xiao;Yingying Zhan;Xiuyun Wang;Chak-tong Au;Lilong Jiang
通讯作者:Lilong Jiang
DOI:10.1016/j.jhazmat.2020.123233
发表时间:2020-06
期刊:Journal of hazardous materials
影响因子:13.6
作者:Yi Liu;Tianhua Zhang;Shusheng Li;Kai Zhang;Xiuyun Wang;Y. Zhan;Ying Zheng;Lilong Jiang
通讯作者:Yi Liu;Tianhua Zhang;Shusheng Li;Kai Zhang;Xiuyun Wang;Y. Zhan;Ying Zheng;Lilong Jiang
基于结构化碱中心的高效COS水解催化剂设计制备及其反应动力学研究
  • 批准号:
    --
  • 项目类别:
    面上项目
  • 资助金额:
    54万元
  • 批准年份:
    2022
  • 负责人:
    詹瑛瑛
  • 依托单位:
国内基金
海外基金