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.

页岩气矿藏中的甲烷已成为重要的能源。 甲烷在商业上用于通过重整和/或部分氧化生产氢气和液体燃料。尽管人们在催化剂开发方面付出了巨大的努力，但传统的甲烷重整和部分氧化过程仍受到各种固有的限制。拟议的研究旨在研究一种独特的甲烷部分氧化催化剂，这些催化剂具有鲁棒性、活性和高效性。该项目将由北卡罗莱纳州立大学研究小组和以色列内盖夫本古里安大学布莱希纳工业催化中心的研究小组（Moti Herskowitz 博士和 Miron Landau 博士）联合开展。该项目团队旨在设计和表征一类核壳氧化还原催化剂，该催化剂既是活性甲烷部分氧化（POx）催化剂，又是有效晶格氧催化剂。 (O2-) 捐助者。该氧化还原催化剂由用于储存氧气的过渡金属氧化物核、促进氧气/电子传导并抑制初级氧化物烧结/失活的混合离子电子导电壳以及用于甲烷部分氧化的定制表面组成。该催化剂在甲烷POx（步骤1）和用空气补充晶格氧（步骤2）的循环氧化还原模式下运行。拟议的研究将研究（i）氧化还原催化剂中的O2-迁移途径以及许多核和壳材料之间的相相容性； (ii) 核壳催化剂的受控合成和表征； (iii)活性金属分散及反应机理研究。 (iv) 模块化填充床系统中甲烷 POx 的动力学建模和演示。所提出的氧化还原催化剂是独特的，因为嵌入的 O2- 可以在没有蒸汽或氧气的情况下实现有效的甲烷氧化。活性O2-还可以抑制焦炭的形成。钙钛矿壳增加了初级氧化物的耐烧结性。它还为活性金属分散和甲烷活化提供了理想的表面。初步研究表明，核壳氧化还原催化剂具有优异的储氧能力（20 wt.%）和高合成气选择性（96%）、活性（600℃下合成气高产率）和结构稳定性（测试温度高达1100℃）。 除了培训研究生和本科生进行研究之外，还计划通过外展活动让代表性不足群体的高中生参与 STEM。拟议项目响应美国制造倡议，并支持由美国化学工程师学会领导的能源部资助的 RAPID 制造研究所的使命。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和更广泛的影响审查标准进行评估，被认为值得支持。

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

LaNixFe1–xO3−δ as a Robust Redox Catalyst for CO2 Splitting and Methane Partial Oxidation

• DOI: 10.1021/acs.energyfuels.1c02258
• 发表时间: 2021-09
• 期刊: Energy & Fuels
• 影响因子: 5.3
• 作者: Sherafghan Iftikhar;Qiongqiong Jiang;Yunfei Gao;Junchen Liu;Haiming Gu;Luke M. Neal;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