Unprecedented High Activity of One-Dimensional Nickel-Based Coordination Polymer for Ethylene Dimerization

IF 3.7 2区 化学 Q2 CHEMISTRY, APPLIED Applied Organometallic Chemistry Pub Date : 2025-01-29 DOI:10.1002/aoc.70019
Yao Ning, Changlian Li, Bo Zhao, Wenpeng Min, Xinyuan Li, Ying Zhang
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Abstract

Three kinds of one-dimensional nickel-based coordination polymers (1D-S-Ni, 1D-D-Ni, and 1D-M-Ni) with different coordination environments and topological structures were synthesized and evacuated as heterogeneous catalysts for liquid phase slurry reaction of ethylene dimerization. Their crystal structures, morphology, chemical groups, and thermal properties were characterized by PXRD, SEM, FT-IR, TGA, ICP-AES, and EA, respectively. The catalytic performance of these catalysts was examined under various reaction conditions, including the amount of cocatalyst, reaction temperature, and reaction pressure. These catalysts showed high catalytic activity up to 105–106 g/(molNi·h) and high selectivity of butene (C4) over 78% at room temperature and 10 atm pressure. Especially the catalytic activity of 1D-D-Ni was up to 17.1 × 105 g/(molNi·h), exceeding that of most Ni-based heterogeneous catalysts and reaching the level of nickel-based homogeneous catalysts. The stability and cyclic performance of 1D-D-Ni was also assessed. It was observed that the catalyst did not undergo decomposition during the reaction and maintained a high activity level of 12.0 × 105 g/(molNi·h) even after three cycles. 1D-D-Ni has SBU similar to homogeneous nickel-based complex catalyst for ethylene dimerization, indicating that reasonable design of metal nodes is an effective way to synthesize heterogeneous ethylene dimerization catalysts with high catalytic performance.

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一维镍基乙烯二聚化配位聚合物的空前高活性
合成了三种具有不同配位环境和拓扑结构的一维镍基配位聚合物(1D-S-Ni、1D-D-Ni和1D-M-Ni),并将其作为乙烯二聚化液相浆液反应的非均相催化剂。采用PXRD、SEM、FT-IR、TGA、ICP-AES和EA对其晶体结构、形貌、化学基团和热性能进行了表征。考察了这些催化剂在不同反应条件下的催化性能,包括助催化剂用量、反应温度和反应压力。在室温和10atm压力下,这些催化剂的催化活性高达105 ~ 106 g/(molNi·h),丁烯(C4)的选择性超过78%。其中,d - d - ni的催化活性高达17.1 × 105 g/(molNi·h),超过了大多数镍基非均相催化剂,达到了镍基均相催化剂的水平。并对1D-D-Ni的稳定性和循环性能进行了评价。结果表明,该催化剂在反应过程中未发生分解,在3次循环后仍保持12.0 × 105 g/(molNi·h)的高活性水平。1D-D-Ni具有与均相镍基乙烯二聚化配合物催化剂相似的SBU,说明合理设计金属节点是合成具有高催化性能的非均相乙烯二聚化催化剂的有效途径。
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来源期刊
Applied Organometallic Chemistry
Applied Organometallic Chemistry 化学-无机化学与核化学
CiteScore
7.80
自引率
10.30%
发文量
408
审稿时长
2.2 months
期刊介绍: All new compounds should be satisfactorily identified and proof of their structure given according to generally accepted standards. Structural reports, such as papers exclusively dealing with synthesis and characterization, analytical techniques, or X-ray diffraction studies of metal-organic or organometallic compounds will not be considered. The editors reserve the right to refuse without peer review any manuscript that does not comply with the aims and scope of the journal. Applied Organometallic Chemistry publishes Full Papers, Reviews, Mini Reviews and Communications of scientific research in all areas of organometallic and metal-organic chemistry involving main group metals, transition metals, lanthanides and actinides. All contributions should contain an explicit application of novel compounds, for instance in materials science, nano science, catalysis, chemical vapour deposition, metal-mediated organic synthesis, polymers, bio-organometallics, metallo-therapy, metallo-diagnostics and medicine. Reviews of books covering aspects of the fields of focus are also published.
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