在 WS2 封闭原子钯位点上进行乙炔加氢制乙烯的环境条件研究

IF 15.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Nature Communications Pub Date : 2024-11-01 DOI:10.1038/s41467-024-53481-1
Wangwang Zhang, Kelechi Uwakwe, Jingting Hu, Yan Wei, Juntong Zhu, Wu Zhou, Chao Ma, Liang Yu, Rui Huang, Dehui Deng
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引用次数: 0

摘要

环境条件下乙炔加氢制乙烯(AC-AHE)是一种前景广阔的乙烯生产工艺,只需极少的额外能量输入,但由于乙炔和 H2 在室温下难以共同活化,该工艺仍面临巨大挑战。在此,我们报告了一种在硫化钨表面的强硫封闭原子钯物种上的高效 AC-AHE 工艺。该催化剂在 25 oC 时乙炔转化率超过 99%,乙烯选择性高达 70%,在环境条件下乙烯的时空产率达到创纪录的 1123 molC2H4 molPd-1 h-1,几乎是典型 Pd1Ag3/Al2O3 催化剂的四倍,并表现出超过 500 h 的卓越稳定性。我们证明,Pd-S 配位的限制诱导了带正电荷的原子 Pdδ+,这不仅有利于 C2H2 加氢,还能促进 C2H4 解吸,从而在室温下实现 C2H2 向 C2H4 的高转化率,同时抑制向 C2H6 的过度加氢。
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Ambient-condition acetylene hydrogenation to ethylene over WS2-confined atomic Pd sites

Ambient-condition acetylene hydrogenation to ethylene (AC-AHE) is a promising process for ethylene production with minimal additional energy input, yet remains a great challenge due to the difficulty in the coactivation of acetylene and H2 at room temperature. Herein, we report a highly efficient AC-AHE process over robust sulfur-confined atomic Pd species on tungsten sulfide surface. The catalyst exhibits over 99% acetylene conversion with a high ethylene selectivity of 70% at 25 oC, and a record space-time yield of ethylene of 1123 molC2H4 molPd−1 h−1 under ambient conditions, which is nearly four times that of the typical Pd1Ag3/Al2O3 catalyst, and exhibiting superior stability of over 500 h. We demonstrate that the confinement of Pd-S coordination induces positively-charged atomic Pdδ+, which not only facilitates C2H2 hydrogenation but also promotes C2H4 desorption, thereby enabling a high conversion of C2H2 to C2H4 at room temperature while suppressing over-hydrogenation to C2H6.

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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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