Collaborative Research: Rational design of Ni/Ga intermetallic compounds for efficient light alkanes conversion through ammonia reforming

合作研究：合理设计Ni/Ga金属间化合物，通过氨重整实现轻质烷烃的高效转化

• 批准号: 2210868
• 负责人: Tao Li
• 金额: $ 28.27万
• 依托单位: Northern Illinois University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-10-01 至 2025-09-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2210868&HistoricalAwards=false
• 关键词: Collaborative; Research; Rational; design; Ni

The transformation of cheap and abundant light alkanes (from natural gas) could have far-reaching implications on the chemical and energy sectors yet remains a formidable challenge due to the lack of efficient catalysts/catalytic systems. While various processes for alkane transformation to a host of petrochemical products have been extensively studied during the past decades, only steam methane reforming, propane dehydrogenation, and steam ethane noncatalytic cracking are produced at large-scale. This project explores an alternative to current catalytic systems known as ammonia-assisted reforming (ammoreforming) of light alkanes. Ammoreforming involves reacting ammonia (NH3) with a light alkane (such as ethane, C3H8) to produce hydrogen cyanide (HCN – an important industrial chemical) and hydrogen (H2). Significantly, the reaction avoids production of either carbon monoxide or carbon dioxide, thus setting the stage for circular usage of carbon with minimal generation of greenhouse gas. The project will strengthen academic research and educational programs in chemistry/chemical engineering at both Mississippi State University and Northern Illinois University. The project leverages several programs at both institutions aimed at stimulating K-12 students’ interest in STEM careers and providing underrepresented undergraduates opportunities to develop research skills.The project focuses on the design and synthesis of efficient non-noble metal - NixGay intermetallic compound (IMC) based catalysts - by the understanding of the structure/performance relationships and catalytic mechanisms of the ammoreforming of light alkanes. The project focuses on several fundamental aspects of ammoreforming over the IMC catalysts, including (1) understanding the effect of oxalate precursor’s composition on the structure, surface properties, and particle size of the NixGay IMC catalysts and their relationships to the catalytic performance of ethane ammoreforming; (2) understanding the influence of oxalate thermo-decomposition and annealing on the structure and surface properties of the NixGay catalysts and the catalytic performance; (3) elucidating the reaction-induced surface/bulk reconstruction and identifying the surface reaction intermediates and catalytic mechanism. The research will be carried out through the combination of in-situ/operando X-ray characterizations (including XRD, SAXS, and XAS) at the Advanced Photon Source of Argonne National Laboratory, operando-DRIFT-MS, and relaxation type transient experiments.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.

由于缺乏有效的催化剂/催化系统，廉价和丰富的光烷烃（来自天然气）的转化可能对化学和能源部门具有深远的影响。尽管在过去几十年中，烷烃转化为多种石化产品的各种过程已经进行了广泛研究，但在大规模的大规模上只生产了蒸汽甲烷改革，丙烷脱氢和蒸汽，蒸汽，蚀刻非催化性裂纹。项目探讨了当前催化系统的替代品，称为氨辅助的改革（Ampormerforming）轻烷烃。提示涉及与氨（例如乙烷，C3H8）反应氨（NH3），以产生氰化氢（HCN - 重要的工业化学化学化学）和氢（H2）。值得注意的是，该反应避免了生产一氧化碳或二氧化碳的产生，从而为碳循环使用而产生了最小的温室气体的循环使用阶段。该项目将加强密西西比州立大学和北伊利诺伊大学化学/化学工程学的学术研究和教育计划。该项目利用了两个机构的几个计划，旨在刺激K -12学生对STEM职业的兴趣，并提供了不足的本科生来发展研究技能的机会。该项目着重于有效的非差异金属的设计和综合 - 基于基于金属的nixgay基于基于金属的金属化合物（IMC）基于基于基于的基于基于的催化剂 - 通过对结构/核对效果的理解，并具有核对效果的理解。该项目侧重于在IMC催化剂上进行Amporming的几个基本方面，包括（1）了解草酸盐前体的组成对Nixgay IMC催化剂的结构，表面特性和粒径的影响及其与它们与疗程成分的催化性能的关系； （2）了解草酸盐热分解和退火对Nixgay催化剂的结构和表面特性的影响； （3）阐明反应引起的表面/体积重建并识别表面反应中间体和催化机制。这项研究将通过在Argonne国家实验室的先进光子来源，Operando-Drift-MS以及放松类型的暂时性实验的高级光子来源的原位/操作X射线字符（包括XRD，SAXS和XAS）的组合进行。这是NSF的法定任务，并通过评估构成的构建精神来进行评估。