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Advanced 3D Hollow-Out ZnZrO@C Combined with Hierarchical Zeolite for Highly Active and Selective CO Hydrogenation to Aromatics
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-06-05 , DOI: 10.1021/acscatal.0c01418 Yajing Wang 1 , Weiteng Zhan 1 , Zhijie Chen 1 , Jianmin Chen 1 , Xingang Li 2 , Yingwei Li 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-06-05 , DOI: 10.1021/acscatal.0c01418 Yajing Wang 1 , Weiteng Zhan 1 , Zhijie Chen 1 , Jianmin Chen 1 , Xingang Li 2 , Yingwei Li 1
Affiliation
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Herein, we explore a facile “defect-mediated outward contraction” strategy to fabricate three-dimensional (3D) hollow-out ZnZrO@C (HO-ZnZrO@C) materials by carbonizing local defect-engineered multivariate UiO-66(ZnZr) (MTV-UiO-66(ZnZr)). The defects mainly result from geometrical substitution of distinct Zn secondary building units for Zr counterparts on MTV-UiO-66 crystals. The as-synthesized HO-ZnZrO@C catalyst possesses rich surface oxygen vacancies on ultrafine ZnZrO nanoparticles, which are confined in robust 3D hierarchical carbon frameworks with open and successive channels. The HO-ZnZrO@C and hierarchical H-ZSM-5 tandem catalyst prepared by powder mixing not only affords a selectivity of aromatics up to 73.1% but also suppresses the CH4 selectivity down to 3.4% at a CO conversion of 35.2%. Particularly, we achieve a record-high space–time yield of 0.302 g goxide–1 h–1 for methanol-mediated COx hydrogenation to aromatics with high catalytic stability. The 2,6-di-tert-butyl-pyridine adsorption FT-IR results indicate that the powder mixing mode between HO-ZnZrO@C and H-ZSM-5 decreases the number of external Brønsted acid sites on H-ZSM-5, which is beneficial for selective hydrogenation of intermediates to aromatics. Our strategy might open up an avenue for the rational design of highly open hierarchical nanostructures with targeted functionalities for various advanced applications.
中文翻译：
先进的3D空心ZnZrO @ C与分层沸石的结合，可实现高活性和选择性CO加氢制芳烃
本文中，我们探索了一种通过碳化局部缺陷设计的多元UiO-66（ZnZr）来制造三维（3D）空心ZnZrO @ C（HO-ZnZrO @ C）材料的简便的“缺陷介导的向外收缩”策略（ MTV-UiO-66（ZnZr））。缺陷主要是由MTV-UiO-66晶体上不同的Zn二级结构单元对Zr对应物的几何取代所致。合成的HO-ZnZrO @ C催化剂在超细ZnZrO纳米颗粒上具有丰富的表面氧空位，这些空位被限制在具有开放和连续通道的坚固3D分层碳框架中。通过粉末混合制备的HO-ZnZrO @ C和分级H-ZSM-5串联催化剂不仅提供了高达73.1％的芳烃选择性，而且还抑制了CH 4在35.2％的CO转化率下，选择性降至3.4％。特别是，通过甲醇介导的CO x加氢成具有高催化稳定性的芳烃，我们实现了创纪录的0.302 gg氧化物–1 h –1的高时空产率。2,6-二叔丁基吡啶的吸附FT-IR结果表明，HO-ZnZrO @ C和H-ZSM-5之间的粉末混合方式减少了H-ZSM-5上外部布朗斯台德酸位的数量，这对于将中间体选择性氢化为芳烃是有利的。我们的策略可能为合理设计高度开放的分层纳米结构开辟一条途径，该结构具有针对各种高级应用的目标功能。
更新日期：2020-06-05
中文翻译：
先进的3D空心ZnZrO @ C与分层沸石的结合，可实现高活性和选择性CO加氢制芳烃
本文中，我们探索了一种通过碳化局部缺陷设计的多元UiO-66（ZnZr）来制造三维（3D）空心ZnZrO @ C（HO-ZnZrO @ C）材料的简便的“缺陷介导的向外收缩”策略（ MTV-UiO-66（ZnZr））。缺陷主要是由MTV-UiO-66晶体上不同的Zn二级结构单元对Zr对应物的几何取代所致。合成的HO-ZnZrO @ C催化剂在超细ZnZrO纳米颗粒上具有丰富的表面氧空位，这些空位被限制在具有开放和连续通道的坚固3D分层碳框架中。通过粉末混合制备的HO-ZnZrO @ C和分级H-ZSM-5串联催化剂不仅提供了高达73.1％的芳烃选择性，而且还抑制了CH 4在35.2％的CO转化率下，选择性降至3.4％。特别是，通过甲醇介导的CO x加氢成具有高催化稳定性的芳烃，我们实现了创纪录的0.302 gg氧化物–1 h –1的高时空产率。2,6-二叔丁基吡啶的吸附FT-IR结果表明，HO-ZnZrO @ C和H-ZSM-5之间的粉末混合方式减少了H-ZSM-5上外部布朗斯台德酸位的数量，这对于将中间体选择性氢化为芳烃是有利的。我们的策略可能为合理设计高度开放的分层纳米结构开辟一条途径，该结构具有针对各种高级应用的目标功能。
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