NSF-BSF and Manufacturing USA: Lattice Oxygen Assisted Methane Activation for Modular Production of Fischer-Tropsch Ready Syngas

NSF-BSF 和美国制造：晶格氧辅助甲烷活化，用于费托合成气的模块化生产

• 批准号: 1923468
• 负责人: Fanxing Li
• 金额: $ 30.55万
• 依托单位: North Carolina State University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-09-15 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1923468&HistoricalAwards=false
• 关键词: NSF; BSF; Manufacturing; USA; Lattice

Methane from shale gas deposits has become an important energy resource. Methane is commercially used to produce hydrogen and liquid fuels via reforming and/or partial oxidation. Although significant efforts have been devoted to catalyst development, conventional methane reforming and partial oxidation processes are subjected to various intrinsic limitations. The proposed research aims to investigate a unique family of catalysts for partial oxidation of methane that are robust, active, and highly efficient. The project will be carried out jointly by the North Carolina State University research group and a group from the Blechner Center for Industrial Catalysis at the Ben-Gurion University of the Negev in Israel (Drs. Moti Herskowitz and Miron Landau).The project team aims to design and characterize a class of core-shell redox catalysts that are both active methane partial oxidation (POx) catalysts and effective lattice oxygen (O2-) donors. The redox catalyst is composed of a transition metal oxide core for O2- storage, a mixed ionic-electronic conductive shell which facilitates O2-/electron conduction and inhibits primary oxide sintering/deactivation, and a tailored surface for methane partial oxidation. The catalyst is operated under a cyclic redox mode for methane POx (step 1) and lattice oxygen replenishment with air (step 2). The proposed research will investigate (i) O2- migration pathway in the redox catalyst and the phase compatibility between a number of core and shell materials; (ii) controlled synthesis and characterization of core-shell catalysts; (iii) active metal dispersion and reaction mechanism studies. (iv) kinetic modeling and demonstration of methane POx in a modular packed bed system. The proposed redox catalyst is unique since the embedded O2- allows effective methane oxidation without steam or oxygen. The active O2- also inhibits coke formation. The perovskite shell increases the sintering resistance of the primary oxide. It also provides an ideal surface for active metal dispersion and methane activation. Preliminary studies have led to core-shell redox catalysts with excellent oxygen storage capacity (20 w.t.%) and high syngas selectivity (96%), activity (high syngas yields at 600 degrees C) and structural stability (tested up to 1,100 degrees C). In addition to training graduate and undergraduate students in research there are plans to engage high school students from underrepresented groups in STEM through outreach activities. The proposed project is responsive to the Manufacturing USA initiative and supports the mission of the DOE-funded RAPID Manufacturing Institute led by the American Institute of Chemical Engineers.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.

页岩气矿床的甲烷已成为重要的能源。 甲烷用于商业用来通过改革和/或部分氧化产生氢和液体燃料。尽管已大量努力致力于催化剂的发展，但常规的甲烷改革和部分氧化过程受到各种固有局限性。拟议的研究旨在研究独特的催化剂家族，以部分氧化甲烷的部分氧化，这些甲烷具有稳健，活跃且高效。 The project will be carried out jointly by the North Carolina State University research group and a group from the Blechner Center for Industrial Catalysis at the Ben-Gurion University of the Negev in Israel (Drs. Moti Herskowitz and Miron Landau).The project team aims to design and characterize a class of core-shell redox catalysts that are both active methane partial oxidation (POx) catalysts and effective lattice oxygen （O2-）捐助者。氧化还原催化剂由用于O2储存的过渡金属氧化物芯组成，一个混合离子电导传导壳，可促进O2-/电子传导并抑制原代氧化物烧结/失活以及用于甲烷部分氧化的表面。该催化剂是在甲烷痘（步骤1）的环状氧化还原模式下运行的（步骤1），并用空气补充了晶格氧气（步骤2）。拟议的研究将研究（i）O2-氧化还原催化剂中的O2迁移途径以及许多核心和壳材料之间的相位兼容性； （ii）核壳催化剂的控制合成和表征； （iii）主动金属分散和反应机理研究。 （iv）模块化床系统中甲烷痘的动力学建模和演示。提出的氧化还原催化剂是独一无二的，因为嵌入的O2允许无蒸汽或氧气的有效甲烷氧化。活性O2-还抑制焦炭的形成。钙钛矿壳增加了原代氧化物的烧结抗性。它还为有源金属分散和甲烷激活提供了理想的表面。初步研究导致核壳氧化还原催化剂具有出色的氧气储存能力（20 w.t.％）和高合成剂选择性（96％），活性（高合成剂在600摄氏度下产生高度的c）和结构稳定性（测试高达1,100度C）。 除了培训研究生和研究生研究生外，还计划通过外展活动与STEM中代表性不足的小组的高中生吸引高中生。拟议的项目对美国化学工程师研究所领导的DOE资助的快速制造研究所的使命有反应。该奖项反映了NSF的法定任务，并被认为是值得通过基金会的知识分子优点和更广泛影响的审查标准来通过评估来进行评估的。

项目成果

Sorption-enhanced steam reforming of toluene using multifunctional perovskite phase transition sorbents in a chemical looping scheme

• DOI: 10.1088/2515-7655/acdbe9
• 发表时间: 2023-06
• 期刊: Journal of Physics: Energy
• 作者: Leo Brody;Mahe Rukh;R. Cai;Azin Saberi Bosari;R. Schomäcker;Fanxing Li

Hydrogenation of bio-oil-derived oxygenates at ambient conditions via a two-step redox cycle

• DOI: 10.1016/j.xcrp.2023.101506
• 发表时间: 2023-07
• 期刊: Cell Reports Physical Science
• 影响因子: 8.9
• 作者: Chongyan Ruan;Ryota Akutsu;Kunran Yang;Noha M. Zayan;Jian Dou;Junchen Liu;A. Bose;Leo Brody;H. Lamb;Fanxing Li

Ce stabilized Ni–SrO as a catalytic phase transition sorbent for integrated CO 2 capture and CH 4 reforming

Ce 稳定的 Ni−SrO 作为催化相变吸附剂，用于集成 CO 2 捕获和 CH 4 重整

• DOI: 10.1039/d1ta09967a
• 发表时间: 2022
• 期刊: Journal of Materials Chemistry A
• 影响因子: 11.9
• 作者: Gu, Haiming;Gao, Yunfei;Iftikhar, Sherafghan;Li, Fanxing
• 通讯作者: Li, Fanxing

Liquid Metal Shell as an Effective Iron Oxide Modifier for Redox-Based Hydrogen Production at Intermediate Temperatures

• DOI: 10.1021/acscatal.1c02102
• 发表时间: 2021-08
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Iwei Wang;Yunfei Gao;Xijun Wang;R. Cai;C. Chung;Sherafghan Iftikhar;Wei Wang;Fanxing Li

Perovskite-Based Phase Transition Sorbents for Sorption-Enhanced Oxidative Steam Reforming of Glycerol

• DOI: 10.1021/acssuschemeng.2c01323
• 发表时间: 2022-04
• 期刊: ACS Sustainable Chemistry & Engineering
• 作者: Leo Brody;R. Cai;Alajia Thornton;Junchen Liu;Hao Yu;Fanxing Li