Amorphous molybdenum sulfide nanocatalysts simultaneously realizing efficient upgrading of residue and synergistic synthesis of 2D MoS2 nanosheets/carbon hierarchical structures†,Green Chemistry

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Amorphous molybdenum sulfide nanocatalysts simultaneously realizing efficient upgrading of residue and synergistic synthesis of 2D MoS2 nanosheets/carbon hierarchical structures†
Green Chemistry ( IF 9.3 ) Pub Date : 2019-10-01 , DOI: 10.1039/c9gc02855b
Yajing Duan _{1,

2,

3,

4,

5} , Yanglin Liu _{4,

6,

7,

8,

9} , Zhaojun Chen _{1,

2,

3,

4} , Dong Liu _{3,

4,

10,

11} , Enqiang Yu _{4,

12,

13,

14,

15} , Xiaodong Zhang _{1,

2,

3,

4} , Hui Fu _{1,

2,

3,

4} , Jinzhe Fu _{1,

2,

3,

4} , Jiatao Zhang _{4,

8,

16,

17,

18} , Hui Du _{1,

2,

3,

4}

Affiliation

College of Chemistry and Chemical Engineering
Qingdao University
Qingdao
China
College of Physics
School of Computer Science and Technology
BIT
Beijing Institute of Technology
Beijing
State Key Laboratory of Heavy Oil Processing
China University of Petroleum
China Offshore Bitumen Co.
Ltd
China National Offshore Oil Corp
Binzhou
Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications
School of Materials Science & Engineering
Beijing 100081

Slurry-phase hydrocracking employing a dispersed catalyst is an efficient technology for the upgrading of residue to clean fuels. The green synthesis of 2D nanosheet hierarchical composites when carrying out some intrinsic functionalities is interesting for both scientific and technological applications. Herein, we present our effort in simultaneously enhancing the residue upgradation and synergistic fabrication of 2D MoS₂ nanosheets/carbon hierarchical structures based on amorphous molybdenum sulfide nanocatalysts. The amorphous molybdenum sulfide nanocatalysts (MoSx-AM, x ≈ 2.79) are constructed in an inverse microemulsion system and are then either modified by oleic acid to synthesize oleophilic MoSx nanocatalysts (MoSx-OL) or annealed to obtain MoS₂ nanocatalysts with the typical layered structure (denoted as MoSx-AN). Benefiting from the decomposition into 2D MoS₂ nanosheets with a length less than 20 nm during the residue slurry-phase hydrocracking, MoSx-AM and MoSx-OL exhibit superior hydrogenation and anti-coke activity compared with MoSx-AN. X-ray photoelectron spectroscopy and density functional theory (DFT) calculation reveal that the residue macromolecules with a polycyclic aromatic structure and heteroatoms show strong interaction with 2D MoS₂ nanosheets, which disturbs the formation of a layered-structure of MoS₂ and results in isolated 2D MoS₂ nanosheets. The generated 2D MoS₂ nanosheets with abundant active sites lead to the superior performance in residue slurry-phase hydrocracking. These results demonstrate a dispersed nanocatalyst for slurry-phase hydrocracking and also provide a perspective for the anti-coke of petroleum refining. In particular, this process also enabled the dispersed 2D MoS₂ nanosheet/carbon hierarchical structure formation synergistically.

中文翻译：

非晶态硫化钼纳米催化剂可同时实现残留物的有效提纯和2D MoS ₂纳米片/碳分层结构的协同合成†

采用分散催化剂的淤浆相加氢裂化是一种将残渣提质为清洁燃料的有效技术。当执行某些固有功能时，二维纳米片分层复合材料的绿色合成对于科学和技术应用而言都是令人感兴趣的。在这里，我们提出我们的工作，同时基于无定形硫化钼纳米催化剂，同时增强残留物的升级和协同制造2D MoS ₂纳米片/碳分级结构。无定形硫化钼纳米催化剂（MOS X -AM，X ≈2.79）被构造在反相微乳液体系中，然后或者通过油酸改性来合成的MoS亲油性X纳米催化剂（MOSx- OL）或退火以获得具有典型分层结构的MoS ₂纳米催化剂（表示为MoS x -AN）。受益于在残余物淤浆相加氢裂化期间分解成长度小于20 nm的2D MoS ₂纳米片，与MoS x -AN相比，MoS x -AM和MoS x -OL表现出优异的氢化和抗焦炭活性。X射线光电子能谱和密度泛函理论（DFT）计算表明，具有多环芳族结构和杂原子的残留大分子与2D MoS ₂纳米片具有强相互作用，这干扰了MoS ₂层状结构的形成并产生孤立的2D MoS ₂纳米片。生成的具有丰富活性位点的2D MoS ₂纳米片在渣浆相加氢裂化方面具有优异的性能。这些结果证明了用于淤浆相加氢裂化的分散的纳米催化剂，并且也为石油精炼的抗焦化提供了前景。特别地，该过程还使得能够协同地形成分散的2D MoS ₂纳米片/碳分级结构。

更新日期：2020-01-02

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