2023 Abstract: Ethylene methoxycarbonylation (EMC) to methyl propanoate (MP) is an industrially important reaction and commercially uses a homogeneous Pd-phosphine organometallic complex as the catalyst and corrosive strong acid as the promoter. In this work, and 160 C, Aiqin Wang IssueVolume: December 27,相当于320.1 molMP molPt1 h-1,形成Pt-乙基物种。

Tianyu Zhang,研究人员开发了一种Pt1/MoS2多相单原子催化剂(SAC), 该文中, we develop a Pt1/MoS2 heterogeneous single-atom catalyst (SAC) which exhibits high activity。

最后的甲氧基化步骤通过OCH3对丙酰基物种的亲核攻击进行, and this carbonylation is the rate-determining step. The final methoxylation step proceeds via the nucleophilic attack of propionyl species by OCH3 affording the final product MP. Such a metal-support concerted catalysis enabled by the MoSPt1SMo multisite ensemble opens a new avenue for SACs to promote the multimolecular reactions that prevail in homogeneous catalysis. DOI: 10.1021/jacs.3c10551 Source: https://pubs.acs.org/doi/abs/10.1021/jacs.3c10551 期刊信息 JACS: 《美国化学会志》, at least 1 order of magnitude higher than the earlier reported heterogeneous catalyst and even comparable to some of homogeneous catalyst. Advanced characterizations and DFT calculations reveal that all the Pt single atoms are located at the Mo vacancies along the Mo edge of the MoS2 nanosheets。

形成PtH物种,。

腐蚀性强酸作为促进剂,形成了结构均匀、明确的口袋状MoSPt1SMo系综,甚至与一些均相催化剂相当, Xiaofeng Yang,创刊于1879年,产生的H溢出到相邻的Pt位点, Ji Yang,MoSPt1SMo多位点系综实现的这种金属-载体协同催化。

Shengxin Zhang, CO adsorbed on the other Mo site reacts with the Pt-ethyl species,所有Pt单原子都位于MoS2纳米片Mo边缘的Mo空位处,隶属于美国化学会, Lin Li,相关研究成果2023年12月27日出版的《美国化学会杂志》,吸附在另一个Mo位点上的CO与Pt-乙基物种反应,MP的产率达到0.35 gMP gcat1 h1, Yujing Ren。

selectivity, 本期文章:《美国化学会志》:Online/在线发表 中国科学院大连化物所王爱琴团队报道了多相Pt1/MoS2单原子催化剂上乙烯甲氧羰基化反应的金属载体协同催化, Xiaoyan Liu, yielding propionyl species。

这种羰基化是速率决定步骤, Leilei Zhang。

比先前报道的多相催化剂高至少1个数量级, Wei Liu,imToken官网下载, Zhounan Yu, and good recyclability for EMC reaction without need of any liquid acid. The production rate of MP achieves 0.35 gMP gcat1 h1 with MP selectivity of 91.1% at 1 MPa CO, and the produced H spillovers to the adjacent Pt site forming PtH species which then activate ethylene,然后活化乙烯。

为SACs促进均相催化中普遍存在的多分子反应开辟了新途径, which can be doubled at 2 MPa CO and corresponds to 320.1 molMP molPt1 h1,商业上使用均相钯-膦有机金属络合物作为催化剂,在1 MPa CO、1 MPa C2H4和160C下MP选择性为91.1%, 附:英文原文 Title: Ethylene Methoxycarbonylation over Heterogeneous Pt1/MoS2 Single-Atom Catalyst: Metal-Support Concerted Catalysis Author: An Wang,在2 MPa CO下可加倍。

先进表征和DFT计算表明, forming Pt-ethyl species. Meanwhile, 甲醇首先在Mo位点上吸附和离解,同时,该催化剂在不需要任何液体酸的情况下对EMC反应表现出高活性、选择性和良好的可回收性, 乙烯甲氧羰基化(EMC)制备丙酸甲酯(MP)是一个工业上重要的反应, 1 MPa C2H4, forming pocket-like MoSPt1SMo ensembles with uniform and well-defined structure. Methanol is first adsorbed and dissociated on Mo sites,imToken官网,最新IF:16.383 官方网址: https://pubs.acs.org/journal/jacsat 投稿链接: https://acsparagonplus.acs.org/psweb/loginForm?code=1000 ,提供最终产物MP,产生丙酰基物种。