低温等离子体促进Ce1-xCoxO2-δ催化剂的晶格氧活化实现低温下炭烟的高效燃烧

doi:10.1016/S1872-2067(25)64775-9

催化学报 ›› 2025, Vol. 77: 99-109.DOI: 10.1016/S1872-2067(25)64775-9

低温等离子体促进Ce_1-_xCo_xO_2-_δ催化剂的晶格氧活化实现低温下炭烟的高效燃烧

张飞飏^a^,^b^,¹, 陈彦君^a^,^b^,¹, 孙孟尧^a^,^b, 王鹏^b, 苗雨欣^b, 郑中洋^b, 刘诗鑫^b^,^*(), 于学华^b, 赵震^a^,^b^,^*()

^a中国石油大学（北京）理学院, 重质油国家重点实验室, 北京 102249
^b沈阳师范大学化学化工学院, 能源与环境催化研究所, 辽宁沈阳 110034

收稿日期:2025-05-03 接受日期:2025-06-24 出版日期:2025-10-18 发布日期:2025-10-05
通讯作者: *电子信箱: liushixin2008@126.com (刘诗鑫),zhenzhao@cup.edu.cn, zhaozhen1586@163.com (赵震).
作者简介:
¹共同第一作者.
基金资助:
国家重点研发计划(2022YFB3504100);国家自然科学基金(22472106)

Non-thermal plasma to boost lattice oxygen activation in Ce_1-_xCo_xO_2-_δ catalysts for efficient soot combustion at low temperatures

Feiyang Zhang^a^,^b^,¹, Yanjun Chen^a^,^b^,¹, Mengyao Sun^a^,^b, Peng Wang^b, Yuxin Miao^b, Zhongyang Zheng^b, Shixin Liu^b^,^*(), Xuehua Yu^b, Zhen Zhao^a^,^b^,^*()

^aState Key Laboratory of Heavy Oil Processing, College of Science, China University of Petroleum (Beijing), Beijing 102249, China
^bInstitute of Catalysis for Energy and Environment, College of Chemistry and Chemical Engineering, Shenyang Normal University, Shenyang 110034, Liaoning, China

Received:2025-05-03 Accepted:2025-06-24 Online:2025-10-18 Published:2025-10-05
Contact: *E-mail: liushixin2008@126.com (S. Liu), zhenzhao@cup.edu.cn, zhaozhen1586@163.com (Z. Zhao).
About author:¹Contributed equally to this work.
Supported by:
National Key Research and Development Program of China(2022YFB3504100);National Natural Science Foundation of China(22472106)

摘要/Abstract

摘要：

柴油机尾气排放的炭烟颗粒物是雾霾形成和PM_2.5浓度升高的关键污染源. 柴油发动机的炭烟颗粒物排放主要集中在其冷启动和怠速阶段, 此时排气温度仅为100-200 °C. 然而, 受限于吸附氧和晶格氧固有的高活化能垒以及活性氧物种(ROSs)缓慢的迁移速率, 即使使用Pt/Pd催化剂, 传统的热催化炭烟燃烧也难以在低温下实现炭烟颗粒物的快速消除. 因此, 急需研发低成本的低温炭烟催化氧化技术, 以满足柴油机尾气炭烟颗粒物超低排放的需求.

低温等离子体(NTP)与催化剂的协同作用能够在温和条件下促进催化剂表面吸附氧和晶格氧的活化, 从而突破传统热催化的局限性. 目前, 已报道的NTP协同催化剂主要关注于对催化剂表面吸附氧的活化利用, 而对晶格氧的利用研究则较少, 低温下反应氧物种生成速率较低, 导致炭烟消除速率和CO₂选择性偏低. 因此, 我们提出通过调控催化剂表面活性位结构以增加对NTP能量的利用效率, 从而显著提高反应氧物种的低温生成速率. 本文通过Co原子掺杂调控氧化铈表面晶格氧和吸附氧的活化能垒, 利用NTP-Ce_1-_xCo_xO_2-_δ协同催化实现表面吸附氧和晶格氧同步双活化, 显著提高了低温下炭烟催化燃烧速率和CO₂选择性. 200 °C和放电功率为4.3 W的条件下, NTP-Ce_0.8Co_0.2O_2-_δ表现出最高的炭烟催化燃烧速率(10 min内炭烟转化率高于90%)和CO₂选择性(99.0%), 其最大能量效率为14.7 g kWh^-1, 是已报道最高能量效率的2倍. 当放电功率提升至6.3 W时, 无需外部加热, 也能实现炭烟快速消除, 炭烟转化率、最大能量效率和CO₂选择性分别为92.1%, 6.1 g kWh^-1和97.5%. 此外, Ce_0.8Co_0.2O_2-_δ具有良好的稳定性和耐水性. 氧同位素示踪实验证实了Ce_0.8Co_0.2O_2-_δ催化剂中的晶格氧被NTP活化且在炭烟低温燃烧中起主要作用, 而吸附氧活化则提高了晶格氧消耗后的补充速率, 晶格氧的补充速率是反应速率的速控步骤. 系统表征和理论计算结果表明, Co掺杂进入CeO₂晶格形成Co-Ce-O固溶体, Co-O-Ce是NTP-催化剂协同催化炭烟燃烧的主要活性位点. 此外, 非对称表面Ce-O-Co构型的晶格氧呈现“易释放-易补充”的动态平衡特性, 实现了低温下炭烟的快速燃烧.

综上所述, 本工作揭示了Ce_1-_xCo_xO_2-_δ催化剂的非对称Ce-O-Co构型不仅有利于NTP促进晶格氧低温活化, 也有利于NTP促进吸附氧活化补充消耗的晶格氧, 这种动态平衡机制显著提高了催化剂对NTP能量利用效率, 为适配NTP环境的高效催化剂的设计提供了新思路.

关键词: 活性氧物种, 晶格氧, 非对称Ce-O-Co结构, 低温等离子体, 炭烟燃烧

Abstract:

Effective lattice oxygen (O_latt) activation at low temperatures has long been a challenge in catalytic oxidation reactions. Traditional thermal catalytic soot combustion, even with Pt/Pd catalysts, is inefficient at exhaust temperatures below 200 °C, particularly under conditions of frequent idling. Herein, we report an effective strategy utilizing non-thermal plasma (NTP) to activate O_latt in Ce_1-_xCo_xO_2-_δ catalysts, achieving dramatic enhancement of the soot combustion rate at low temperatures. At 200 °C and 4.3 W (discharge power, P_dis), NTP-Ce_0.8Co_0.2O_2-_δ achieved 96.9% soot conversion (X_C), 99.0% CO₂ selectivity (S(CO₂)) and a maximum energy conversion efficiency (E_max) of 14.7 g kWh^-1. Compared with previously reported results, NTP-Ce_0.8Co_0.2O_2-_δ exhibits the highest S(CO₂) and E_max values. Remarkably, even without heating, X_C, E_max, and S(CO₂) reached 92.1%, 6.1 g kWh^-1, and 97.5%, respectively, at 6.3 W (P_dis). The results of characterization and theoretical calculation demonstrated that Co dopes into the CeO₂ crystal lattice and forms an asymmetric Ce-O-Co structure, making oxygen “easy come, easy go”, thereby enabling the rapid combustion of soot over NTP-Ce_0.8Co_0.2O_2-_δ. This study highlights the great potential of NTP for activating O_latt and provides valuable insights into the design of efficient NTP-adapted catalysts for oxidation reactions.

Key words: Reactive oxygen species, Lattice oxygen, Asymmetric Ce-O-Co structure, Non-thermal plasma, Soot combustion

张飞飏, 陈彦君, 孙孟尧, 王鹏, 苗雨欣, 郑中洋, 刘诗鑫, 于学华, 赵震. 低温等离子体促进Ce_1-_xCo_xO_2-_δ催化剂的晶格氧活化实现低温下炭烟的高效燃烧[J]. 催化学报, 2025, 77: 99-109.

Feiyang Zhang, Yanjun Chen, Mengyao Sun, Peng Wang, Yuxin Miao, Zhongyang Zheng, Shixin Liu, Xuehua Yu, Zhen Zhao. Non-thermal plasma to boost lattice oxygen activation in Ce_1-_xCo_xO_2-_δ catalysts for efficient soot combustion at low temperatures[J]. Chinese Journal of Catalysis, 2025, 77: 99-109.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64775-9

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Fig. 1. (a) XRD patterns of Ce1-xCoxO2-δ catalysts. (b) Magnified XRD patterns of Ce1-xCoxO2-δ catalysts in the range from 27° to 30°. (c) Raman spectra of Ce1-xCoxO2-δ catalysts. (d) HRTEM images of Ce0.8Co0.2O2-δ catalyst. (e) HRTEM images of Ce0.6Co0.4O2-δ catalyst. (f) O2-TPD profiles of Ce1-xCoxO2-δ catalysts.

Fig. 2. (a) Time-dependent curves of COx concentrations of NTP-Ce1-xCoxO2-δ (x = 0, 0.2, and 1). (b) XC of NTP-Blank and NTP-Ce1-xCoxO2-δ (x = 0, 0.2, 0.4, and 1) as a function of reaction time. (c) XC and S(CO2) of NTP-Blank and NTP-Ce1-xCoxO2-δ/-HCl. (d) The stability of Ce0.8Co0.2O2-δ catalyst. (e) Emax of the NTP-Ce1-xCoxO2-δ (200 °C, Pin = 13 W and 10% O2/N2). (f) Water resistance of Ce1-xCoxO2-δ (x = 0.1-0.4) catalysts (200 °C, Pin = 13 W and 10% O2/10% H2O/N2). (g) Effect of NO concentration (Pin = 13 W and 150 °C) on the catalytic activity of Ce0.8Co0.2O2-δ catalyst. (h) Effect of Pdis (without heating and 10% O2/N2) and reaction temperature (Pin = 13 W and 10% O2/N2) on the catalytic activity of Ce0.8Co0.2O2-δ catalyst. (i) XRD patterns of Ce1-xCoxO2-δ/-HCl (x = 0.2, 0.4).

Fig. 3. (a-c) Isothermal plasma isotope exchange reactions on Ce1-xCoxO2-δ (x = 0, 0.2 and 1) catalysts without soot (a) and with soot (b,c) (Pin = 13 W). (d) XRD patterns of Ce1-xCoxO2-δ, Ce1-xCoxO2-δ-R and Ce1-xCoxO2-δ-S catalysts (x = 0 and 0.2). (e) Raman spectra of Ce1-xCoxO2-δ, Ce1-xCoxO2-δ-R and Ce1-xCoxO2-δ-S catalysts (x = 0 and 0.2). (f) Ce 3d XPS spectra of Ce0.8Co0.2O2-δ, Ce0.8Co0.2O2-δ-R and Ce0.8Co0.2O2-δ-S catalysts (Ce3+: Ce3+/(Ce3+ + Ce4+) × 100). (Ce1-xCoxO2-δ-R and Ce1-xCoxO2-δ-S are the used catalysts in soot combustion by NTP-catalyst without gas-phase oxygen and regenerated by NTP in 10% O2/N2 flow, respectively.)

Fig. 4. Structural configurations of CeO2 (a), Co-CeO2 (b), CeO2-Vo (c), and Co-CeO2-Vo (d). Energy of formation of the second Vo by the direct (e) and migration (f) removal processes. (g) Energy profiles of the O2 supplement for CeO2 and Co-CeO2. Electron localization function (ELF) maps of CeO2 (h) and Co-CeO2 (i). Projected crystal orbital Hamilton populations (pCOHP) for CeO2 (j) and Co-CeO2 (k) (red, yellow, and blue balls represent O, Ce, and Co atoms, respectively). (l) Synergistic catalytic mechanism of the NTP-Ce1-xCoxO2-δ hybrid for soot oxidation.

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低温等离子体促进Ce_1-_xCo_xO_2-_δ催化剂的晶格氧活化实现低温下炭烟的高效燃烧

Non-thermal plasma to boost lattice oxygen activation in Ce_1-_xCo_xO_2-_δ catalysts for efficient soot combustion at low temperatures

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低温等离子体促进Ce1-xCoxO2-δ催化剂的晶格氧活化实现低温下炭烟的高效燃烧

Non-thermal plasma to boost lattice oxygen activation in Ce1-xCoxO2-δ catalysts for efficient soot combustion at low temperatures

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低温等离子体促进Ce_1-_xCo_xO_2-_δ催化剂的晶格氧活化实现低温下炭烟的高效燃烧

Non-thermal plasma to boost lattice oxygen activation in Ce_1-_xCo_xO_2-_δ catalysts for efficient soot combustion at low temperatures