RUI: CAS: Carbon Dioxide Hydrogenation to Light Olefins over Carbon Nanosphere Encapsulated Metal/Metal Carbide Core-Shell Catalysts

RUI：CAS：碳纳米球封装金属/金属碳化物核壳催化剂上二氧化碳加氢生成轻质烯烃

• 批准号: 1955521
• 负责人: Cheng Zhang
• 金额: $ 26.5万
• 依托单位: Long Island University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-09-01 至 2023-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1955521&HistoricalAwards=false
• 关键词: RUI; CAS; Carbon; Dioxide; Hydrogenation

Carbon-rich fossil fuels, such as coal, oil, and natural gas, have been heavily utilized to power human civilization. This has resulted in massive emissions of carbon dioxide (CO2), a potent greenhouse gas, to the environment. There is an urgent need to mitigate the negative impacts of these emissions on the environment. Efficient utilization of CO2 to produce chemicals and fuels is one potential solution. This research project is examining the conversion of CO2 to light olefins. Olefins are important chemicals and raw materials heavily used for the packaging, plastic processing, construction, and textile industries. The huge market demand for light olefins offers a great opportunity for this project to significantly impact CO2 utilization technology. While significant advances have been made, considerable challenges remain for the discovery and development of practical catalysts for this transformation. In this project, Professor Cheng Zhang of the Long Island University (Post), New York is developing a new approach using carbon nanosphere (CNS) encapsulated metal catalysts for CO2 conversion to light olefins. Dr. Zhang is studying CNS encapsulated iron-cobalt catalysts and investigating their fundamental reaction mechanisms. These fundamental insights are being used to design new catalysts that perform much more efficiently. Dr. Zhang is actively engaged in training the next generation of undergraduates in chemistry education and research. Dr. Zhang’s lab involves diverse students from various majors in this interdisciplinary setting. This research is further serving as a platform to inspire students from underrepresented groups to become scientists.With the funding from the Chemical Catalysis Program of the Division of Chemistry, Dr. Zhang of the Long Island University (Post), New York is developing fundamental understanding of a class of new catalysts, carbon nanosphere (CNS) encapsulated metal/metal carbide nanoparticle core-shell structures, for catalytic CO2 conversion to light olefins. This project is significant in studying the composition, structure, and catalytic performances of CNS encapsulated metal/metal carbide catalysts by integrating synthesis, testing, and characterization of the catalysts with multiple compositional and structural variables. Specifically, the CNS encapsulated Fe catalyst provides an intriguing catalytic performance for CO2 conversion to light olefins. A variety of characterization instruments including in-situ time-resolved X-ray diffraction (TR-XRD), ex-situ x-ray absorption near edge structure spectroscopy (XANES), and high-resolution transmission electron microscopy (HRTEM) are utilized to achieve a fundamental understanding of the reaction pathways and the confinement effect that contributes to the superior performance. Furthermore, with CNS serves as a nanocontainer, the encapsulated Fe-Co catalyst is expected to exhibit enhanced catalytic performances due to the synergistic effect of the bimetals, together with the unique confinement effect of CNS. By synthetically changing the relative shell thickness and core dimeter, a core-shell nano-environment of encapsulated active Fe/Co core species in the CNS shells provides an ideal and practical model system to explore the fundamentals of structural variables on the role of confinement in catalysis. This project has the dual impact of removing CO2 from the atmosphere while generating desired commercial products. Dr. Zhang incorporates undergraduate research and education as a very significant component. Dr. Zhang is developing a training-learning platform that allows undergraduate and high school students to gain valuable skills in synthesis, catalyst evaluation techniques and basic characterization, in conjunction with their quantitative and critical thinking skills, which paves the way for their future career development.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

煤炭，石油和天然气等富含碳的化石燃料已被大量用于为人类文明提供动力。这导致了对环境的二氧化碳（CO2）的大量排放。迫切需要减轻这些排放对环境的负面影响。有效利用CO2生产化学物质和燃料是一种潜在的解决方案。该研究项目正在研究二氧化碳向光烯烃的转化。烯烃是重要的化学品和原材料，用于包装，塑料加工，建筑和纺织工业。对光烯烃的巨大市场需求为该项目提供了一个很好的机会，可以显着影响二氧化碳利用技术。尽管已经取得了重大进展，但对于这种转变的实践催化剂的发现和开发仍然存在巨大挑战。在该项目中，纽约长岛大学（POST）的郑张教授正在使用碳纳米球（CNS）封装的金属催化剂来开发一种新方法，以转换为烯烃。张博士正在研究中枢神经系统封装的铁 - 铜催化剂并研究其基本反应机制。这些基本的见解被用来设计出更有效的新催化剂。张博士积极从事化学教育和研究领域的下一代大学生的培训。张博士的实验室在这个跨学科的环境中涉及来自各个专业的学生。这项研究进一步是一个平台，以激发代表性不足的群体的学生成为科学家。 With the funding from the Chemical Catalysis Program of the Division of Chemistry, Dr. Zhang of the Long Island University (Post), New York is developing fundamental understanding of a class of New catalysts, carbon nanosphere (CNS) encapsulated metal/metal carbide nanoparticle core-shell structures, for catalytic CO2 conversion to light olefins.该项目对于研究中枢神经系统封装金属/金属碳化物催化剂的组成，结构和催化性能很重要，通过将催化剂与多个组成和结构变量的合成，测试和表征整合在一起。具体而言，CNS封装的FE催化剂为二氧化碳转化为光烯烃提供了有趣的催化性能。各种表征仪器，包括原位时间分辨X射线衍射（TR-XRD），EX-Situ X射线抽象近边缘结构光谱（XANES）和高分辨率的传输电子显微镜（HRTEM），可用于实现对反应途径和限制性效果的基本了解。此外，使用CNS充当纳米结构剂，预计封装的Fe-CO催化剂有望暴露由于双甲基的协同作用以及CNS的独特限制作用，因此会暴露出增强的催化性能。通过合成改变相对的壳厚度和核心尺寸，CNS壳中包裹的活性Fe/Co核心物种的核心壳纳米环境提供了一个理想且实用的模型系统，以探索结构变量对催化中约束作用的基础。该项目在产生所需的商业产品的同时，从大气中删除CO2的双重影响。张博士将本科研究和教育纳入了非常重要的组成部分。张博士正在开发一个培训学习平台，该平台使本科生和高中生能够在合成，催化剂评估技术和基本表征方面获得宝贵的技能，并结合他们的定量和批判性思维能力，为他们未来的职业发展铺平了道路，这对NSF的法定任务进行了评估，并通过评估了良好的范围。

项目成果

CO2 to Value-Added Chemicals: Synthesis and Performance of Mono- and Bimetallic Nickel–Cobalt Nanofiber Catalysts

• DOI: 10.3390/catal13061017
• 发表时间: 2023-06
• 期刊: Catalysts
• 影响因子: 3.9
• 作者: John Schossig;Akash Gandotra;Kevin Arizapana;Daniel Jochen Weber;Michael Wildy;Wanying Wei;Kai Xu;L. Yu;R. Chimenti;Islam M. Mantawy;D. Hyun;Wenshuai Chen;Cheng Zhang;Ping Lu

Recent Advances in the Mitigation of the Catalyst Deactivation of CO2 Hydrogenation to Light Olefins

• DOI: 10.3390/catal11121447
• 发表时间: 2021-11
• 期刊: Catalysts
• 影响因子: 3.9
• 作者: D. Weber;T. He;Matthew Wong;Christian Moon;Axel Zhang;Nicole Foley;Nicholas J. Ramer;Cheng Zhang-C

Utilizing bimetallic catalysts to mitigate coke formation in dry reforming of methane

利用双金属催化剂减少甲烷干重整中的焦炭形成

• DOI: 10.1016/j.jechem.2021.11.041
• 发表时间: 2022
• 期刊: Journal of Energy Chemistry
• 影响因子: 13.1
• 作者: Sasson Bitters, Jaylin;He, Tina;Nestler, Elizabeth;Senanayake, Sanjaya D.;Chen, Jingguang G.;Zhang, Cheng
• 通讯作者: Zhang, Cheng

Hollow Graphitic Carbon Nanospheres Synthesized by Rapid Pyrolytic Carbonization

• DOI: 10.4028/www.scientific.net/jnanor.68.1
• 发表时间: 2021-06
• 期刊: Journal of Nano Research
• 影响因子: 1.7
• 作者: Cheng Zhang;Qingwen Gao;L. Jiao;Laura Bogen;N. Forte;Elizabeth Nestler