Mechanistic in situ insights into the formation, structural and catalytic aspects of the La2NiO4 intermediate phase in the dry reforming of methane over Ni-based perovskite catalysts

Nezhad Parastoo Delir Kheyrollahi; Bekheet Maged F.; Bonmassar Nicolas; Schlicker Lukas; Gili Albert; Kamutzki Franz; Gurlo Aleksander; Doran Andrew; Gao Yuanxu; Heggen Marc; Schwarz Sabine; Bernardi Johannes; Niaei Aligholi; Farzi Ali; Klotzer Bernhard; Penner Simon

首页> 外文期刊>Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications >Mechanistic in situ insights into the formation, structural and catalytic aspects of the La2NiO4 intermediate phase in the dry reforming of methane over Ni-based perovskite catalysts

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Mechanistic in situ insights into the formation, structural and catalytic aspects of the La2NiO4 intermediate phase in the dry reforming of methane over Ni-based perovskite catalysts

机译：在Ni基钙钛矿催化剂中甲烷干燥重整中La2NiO4中间相的形成，结构和催化方面的机械洞察力

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We focus on the stability and bulk/surface structural properties of the Ruddlesden-Popper phase La2NiO4 and their consequences for dry reforming of methane (DRM) activity. Fuelled by the appearance as a crucial intermediate during in situ decomposition of highly DRM-active LaNiO3 perovskite structures, we show that La2NiO4 can be equally in situ decomposed into a Ni/La2O3 phase offering CO2 capture and release necessary for DRM activity, albeit at much higher temperatures compared to LaNiO3. Decomposition in hydrogen also leads to an active Ni/La2O3 phase. In situ X-ray diffraction during DRM operation reveals considerable coking and encapsulation of exsolved Ni, yielding much smaller Ni crystallites compared to on LaNiO3, where coking is virtually absent. Generalizing the importance of intermediate Ruddlesden-Popper phases, the in situ decomposition of Labased perovskite structures yields several obstacles due to the high stability of both the parent perovskite and the Ruddlesden-Popper structures and the occurrence of parasitic structures.

机译：我们主要研究Ruddlesden-Popper相La2NiO4的稳定性和体/表面结构特性，以及它们对甲烷干重整（DRM）活性的影响。在高DRM活性的LaNiO3钙钛矿结构原位分解过程中，La2NiO4作为一种关键中间体的出现，使我们发现La2NiO4可以同样地原位分解为Ni/La2O3相，提供DRM活性所需的CO2捕获和释放，尽管温度比LaNiO3高得多。在氢中分解也会产生活性Ni/La2O3相。DRM操作期间的原位X射线衍射显示出出溶出镍的大量结焦和包裹，与LaNiO3相比，产生的镍微晶要小得多，而LaNiO3上几乎没有结焦。概括中间Ruddlesden-Popper相的重要性，由于母体钙钛矿和Ruddlesden-Popper结构的高稳定性以及寄生结构的出现，实验室钙钛矿结构的原位分解会产生一些障碍。

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《Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications》 |2021年第1期|共11页
作者
Nezhad Parastoo Delir Kheyrollahi; Bekheet Maged F.; Bonmassar Nicolas; Schlicker Lukas; Gili Albert; Kamutzki Franz; Gurlo Aleksander; Doran Andrew; Gao Yuanxu; Heggen Marc; Schwarz Sabine; Bernardi Johannes; Niaei Aligholi; Farzi Ali; Klotzer Bernhard; Penner Simon;
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作者单位

Univ Tabriz Dept Chem Engn Reactor &

Catalyst Res Lab Tabriz Iran;

Tech Univ Berlin Fachgebiet Keram Werkstoffe Chair Adv Ceram Mat Inst Werkstoffwissensch &

Technol Hardenbergstr 40 D-10623 Berlin Germany;

Univ Innsbruck Dept Phys Chem Innrain 52c A-6020 Innsbruck Austria;

Tech Univ Berlin Fachgebiet Keram Werkstoffe Chair Adv Ceram Mat Inst Werkstoffwissensch &

Technol Hardenbergstr 40 D-10623 Berlin Germany;

Tech Univ Berlin Fachgebiet Keram Werkstoffe Chair Adv Ceram Mat Inst Werkstoffwissensch &

Technol Hardenbergstr 40 D-10623 Berlin Germany;

Tech Univ Berlin Fachgebiet Keram Werkstoffe Chair Adv Ceram Mat Inst Werkstoffwissensch &

Technol Hardenbergstr 40 D-10623 Berlin Germany;

Tech Univ Berlin Fachgebiet Keram Werkstoffe Chair Adv Ceram Mat Inst Werkstoffwissensch &

Technol Hardenbergstr 40 D-10623 Berlin Germany;

Lawrence Berkeley Natl Lab Adv Light Source Berkeley CA 94720 USA;

Forschungszentrum Julich Ernst Ruska Ctr Mikroskopie &

Spektroskopie Elekt D-52425 Julich Germany;

Forschungszentrum Julich Ernst Ruska Ctr Mikroskopie &

Spektroskopie Elekt D-52425 Julich Germany;

TU Wien Univ Serv Ctr Transmiss Electron Microscopy Wiedner Hauptstr 8-10 A-1040 Vienna Austria;

TU Wien Univ Serv Ctr Transmiss Electron Microscopy Wiedner Hauptstr 8-10 A-1040 Vienna Austria;

Univ Tabriz Dept Chem Engn Reactor &

Catalyst Res Lab Tabriz Iran;

Univ Tabriz Dept Chem Engn Reactor &

Catalyst Res Lab Tabriz Iran;

Univ Innsbruck Dept Phys Chem Innrain 52c A-6020 Innsbruck Austria;

Univ Innsbruck Dept Phys Chem Innrain 52c A-6020 Innsbruck Austria;

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正文语种 eng
中图分类物理化学（理论化学）、化学物理学;
关键词
CO lt; sub gt; 2 lt; sub gt; -activation; B-site exsolution; Polymorphism; In situ decomposition;

机译：CO;sub;2;sub-激活;B位溶出液;多态性;原位分解;

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专利

1. Catalytic performance of perovskite-like oxide doped cerium (La2-xCexCoO4±y) as catalysts for dry reforming of methane [J] . Yukun Bai, Yuqi Wang, Weijian Yuan, 中国化学工程学报（英文版） . 2019,第002期
2. Kinetic simulation of oxidative coupling of methane over perovskite catalyst by genetic algorithm： Mechanistic aspects [J] . Nastaran Razmi Farooji, Ali Vatani, Shahrnaz Mokhtarit 天然气化学杂志：英文版 . 2010,第004期
3. Kinetic simulation of oxidative coupling of methane over perovskite catalyst by genetic algorithm:Mechanistic aspects [J] . Nastaran Razmi Farooji, Ali Vatani, Shahrnaz Mokhtari 天然气化学（英文版） . 2010,第004期
4. Improvement of catalytic stability for CO2 reforming of methane by copper promoted Ni-based catalyst derived from layered-double hydroxides [J] . Bing Li, Zhenxin Xu, Fangli Jing, 天然气化学（英文版） . 2016,第006期
5. Improvement of catalytic stability for CO2 reforming of methane by copper promoted Ni-based catalyst derived from layered-double hydroxides [J] . Bing Li, Zhenxin Xu, Fangli Jing, 能源化学：英文版 . 2016,第006期
6. Steering the Methane Dry Reforming Reactivity of Ni/La2O3 Catalysts by Controlled In Situ Decomposition of Doped La2NiO4 Precursor Structures [J] . Maged F. Bekheet, Parastoo Delir Kheyrollahi Nezhad, Nicolas Bonmassar, ACS catalysis . 2021,第1期

机译：通过对掺杂La2NiO4前体结构的原位分解，通过控制Ni / La2O3催化剂的甲烷干重改性反应性
7. Low-temperature catalytic CO2 dry reforming of methane on Ni-based catalysts: A review [J] . Wang Ye, Yao Lu, Wang Shenghong, Fuel Processing Technology . 2018,第期

机译：Ni基催化剂对甲烷的低温催化CO2干燥重整：综述
8. Catalytic activity and effect of modifiers on Ni-based catalysts for the dry reforming of methane [J] . Maria Martha Barroso-Quiroga, Adolfo Eduardo Castro-Luna International journal of hydrogen energy . 2010,第11期

机译：甲烷干重整制镍基催化剂的催化活性和改性剂的作用
9. Reaction Kinetics of Catalytic Dry Reforming of Methane on Spinel-Derived Nickel Catalyst at Low-Temperature Using an in-Situ Stagnation-Flow Reactor [C] . Yonggyun Bae, Jongsup Hong Pacific Rim Meeting on Electrochemical and Solid-State Science . 2020

机译：用原位停滞 - 流动反应器在低温下尖晶石衍生镍催化剂催化干重整的反应动力学
10. Directly observing catalytic intermediates of methane dry reforming (MDR) on model Ni(111) catalyst via in operando surface techniques [D] . Yuan, Kaidi 2017

机译：在Operando表面技术中直接观察甲烷干重整（MDR）催化中间体甲烷干重整（MDR）的催化剂
11. Highly active dry methane reforming catalysts with boosted in situ grown Ni-Fe nanoparticles on perovskite via atomic layer deposition [O] . Sangwook Joo, Arim Seong, Ohhun Kwon, 2020

机译：高活性干燥甲烷重整催化剂通过原子层沉积在钙钛矿上升压原位生长的Ni-Fe纳米粒子
12. Steering the Methane Dry Reforming Reactivity of Ni/La2O3 Catalysts by Controlled In Situ Decomposition of Doped La2NiO4 Precursor Structures [O] . Maged F. Bekheet, Parastoo Delir Kheyrollahi Nezhad, Nicolas Bonmassar, 2020

机译：通过对掺杂La2NiO4前体结构的原位分解来转向Ni / La2O3催化剂的甲烷干重改性反应性
13. Ab Initio Studies of Coke Formation on Ni Catalysts during Methane Reforming (Final Report, September 26, 2002-November 25, 2005) [R] . Sholl, D. S. 2006

机译：甲烷重整过程中Ni催化剂上焦炭形成的从头算研究（最终报告，2002年9月26日 - 2005年11月25日）

Mechanistic in situ insights into the formation, structural and catalytic aspects of the La2NiO4 intermediate phase in the dry reforming of methane over Ni-based perovskite catalysts

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