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.

富含碳的化石燃料，如煤、石油和天然气，已被大量用于为人类文明提供动力。这导致二氧化碳（CO2）（一种强有力的温室气体）大量排放到环境中。迫切需要减轻这些排放对环境的负面影响。有效利用二氧化碳生产化学品和燃料是一个潜在的解决方案。该研究项目正在研究将CO2转化为轻质烯烃。烯烃是重要的化学品和原材料，大量用于包装、塑料加工、建筑和纺织工业。轻质烯烃的巨大市场需求为该项目提供了一个巨大的机会，以显着影响二氧化碳利用技术。虽然已经取得了重大进展，但在发现和开发用于这种转化的实用催化剂方面仍然存在相当大的挑战。在这个项目中，纽约长岛大学（Post）的Cheng Zhang教授正在开发一种新的方法，使用碳纳米球（CNS）封装的金属催化剂将CO2转化为轻烯烃。张博士正在研究CNS封装的铁钴催化剂，并研究其基本反应机理。这些基本的见解被用来设计新的催化剂，更有效地执行。张博士积极致力于培养下一代化学教育和研究的本科生。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不同学生。在化学系化学催化项目的资助下，纽约长岛大学（Post）的Zhang博士正在开发一类新催化剂的基本理解，碳纳米球（CNS）封装的金属/金属碳化物纳米颗粒核壳结构，用于将CO2催化转化为轻质烯烃。该项目是重要的在研究CNS封装的金属/金属碳化物催化剂的组成，结构和催化性能，通过集成的合成，测试和表征的催化剂与多个组成和结构变量。具体地，CNS包封的Fe催化剂提供了用于将CO2转化为轻质烯烃的令人感兴趣的催化性能。各种表征仪器，包括原位时间分辨X射线衍射（TR-XRD），非原位X射线吸收近边结构光谱（XANES），和高分辨率透射电子显微镜（HRTEM）被用来实现的反应途径和限制效应，有助于上级性能的基本理解。此外，CNS作为纳米容器，由于双金属的协同效应以及CNS的独特限制效应，预期封装的Fe-Co催化剂表现出增强的催化性能。通过综合改变壳层相对厚度和核的直径，在CNS壳层中形成的Fe/Co核活性物种的核-壳纳米环境，为探索结构变量对禁闭催化作用的基本原理提供了一个理想而实用的模型体系。该项目具有双重影响，即从大气中去除二氧化碳，同时产生所需的商业产品。张博士将本科研究和教育作为一个非常重要的组成部分。张博士正在开发一个培训学习平台，让本科生和高中生获得合成，催化剂评估技术和基本表征方面的宝贵技能，结合他们的定量和批判性思维技能，该奖项反映了NSF的法定使命，并通过使用基金会的智力价值进行评估，被认为值得支持和更广泛的影响审查标准。

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

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

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