Catalysts
·
2025
·Vol. 15
·期 3
·295
·
IF 4
Weijie Kong,Wenhui Zhang,Yiming Wang,Xin Chen,Yongjian Ai,Zenan Hu,Hong-Bin Sun
The process of directly using atmospheric H2for the catalytic semi-hydrogenation of alkynes to alkenes has significant applications in the polyolefin industry. Herein, we report a facile approach to synthesize a hierarchical carbon-encapsulated Pd catalyst for the highly selective semi-hydrogenation of nitrophenylacetylene. The catalyst featured a structure of (Pd@NG)/(Pd@C), which demonstrated that an oligo-layer of nitrogen-doped graphene (NG)-encapsulated Pd particles are supported on the carbon matrix, semi-embedded by another type of Pd particle. The catalyst, named Pd@NC, achieved 99% selectivity for nitrostyrene at 97% nitrophenylacetylene conversion and demonstrated an excellent stability. A good selectivity arose from the bridging effect of hierarchical porous carbon, where hydrogen activation and alkyne hemihydrogenation took place on palladium particles and NG, respectively. The NG layer provided excellent protection against the over-hydrogenation of the reaction.
研究领域:
催化化学
·
材料科学
·
纳米技术
·
有机合成
·
工业化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Yangguang Hu,Song Wang,Zifan Jiang,Wanbing Gong,Aobo Chen,Qiaoxi Liu,Guangyu Liu,Zhiqiang Shen,Jingxiang Low,Jun Ma,Jun Jiang,Chao Gao,Yujie Xiong
Selective semihydrogenation of acetylene to ethylene in ethylene-rich gas streams is a significant industrial process for obtaining high-quality polyethylene products. The conventional thermal hydrogenation route requires high temperature (>100 °C), excess H2, and noble metal Pd to achieve satisfactory conversion efficiency. Therefore, the development of a more efficient and economical low-energy method for acetylene semihydrogenation is greatly desired yet challenging. Here, we report a noble-metal-free molecular system consisting of a bioinspired [CoII(N4S2)](ClO4)2 catalyst and a copper photosensitizer, which achieves photocatalytic semihydrogenation of acetylene to ethylene with over 96% selectivity and 96–99.9% conversion under ambient conditions for both pure acetylene and industrially relevant ethylene cofeed (containing 1% acetylene) conditions using water as a proton source. In addition, our catalytic system in deuterium oxide exhibits ability for deuterated ethylene production, which is an important building block for various deuterated polyolefins and chemicals.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Communications
·
2025
·
IF 4.5
Yujie Wang,Jiaying Liu,Yongbo Cui,Meng Liu,Wenxia Chen,Wei Wei,Haifeng Lu,Dongyun Han
The semi-hydrogenation of alkynes with high chemo and regioselectivity represents a significant yet challenging aspect in the synthesis of functionalized alkenes. A straightforward hydrothermal technique was utilized to synthesize amorphous cobalt sulfide polyhedra (CoS x ). This material facilitates the electrocatalytic semi-hydrogenation of terminal alkynes in water, particularly those possessing reducible groups such as C-I, C-Br, C-Cl, and C-O. The process yields impressive results, with a conversion rate of up to 99 % and a selectivity of as high as 95 %. Moreover, it demonstrates a wide substrate scope and excellent compatibility with a variety of functional groups. The high conversion rate of alkynes, coupled with the high selectivity for alkenes, and the catalyst's excellent versatility, collectively underscore the potential of our method.
研究领域:
化学
·
材料科学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Huawei Li,Miao He,Senyao Meng,Ping Wang,Cheng Yang,Jiasai Yao,Zikang Hu,Zhenxing Li
The removal of acetylene (C2H2) impurities from ethylene (C2H4) is a critical step in the production of high-purity C2H4. Due to its low reaction temperature, low energy consumption and high selectivity for C2H4, the electrocatalytic semi-hydrogenation of C2H2 is an ideal method for removing C2H2. Herein, ultrathin two-dimensional (2D) mesoporous holmium oxide nanosheet-stabilized copper nanoparticles (Cu/Ho2O3) for stable and efficient electrocatalytic semi-hydrogenation of C2H2 were prepared through a simple and one-step high-temperature calcination-reduction method. The ultra-thin two-dimensional mesoporous structure of holmium oxide creates abundant coordination defects, improving the faradaic efficiency and durability of copper nanoparticles for catalyzing the semi-hydrogenation of C2H2. The as-prepared Cu/Ho2O3 achieved a C2H4 selectivity of 99.6% and a faradaic efficiency of 98.1% because the presence of oxygen vacancies is conducive to forming electron-rich Cu nanoparticles, thereby promoting the adsorption of electrophilic C2H2 and the desorption of nucleophilic C2H4. Meanwhile, the holmium oxide nanosheet with unsaturated coordination sites can stabilize the Cu nanoparticles, and the faradaic efficiency and current density remain stable for more than 600 minutes. This work offers a promising design strategy for a stable and efficient electrocatalyst for the semi-hydrogenation of C2H2 to C2H4.
研究领域:
材料科学
·
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhenpeng Liu,Zhe Chen,Jun Bu,Wenxiu Ma,Lei Zhang,Hong Zhong,Lin Cheng,Shuangming Li,Tao Wang,Jian Zhang
Compared to their booming thermocatalytic counterparts, electrocatalytic acetylene semihydrogenation still remain stagnant owing to its low activity and poor selectivity. Here, we first explore metal phthalocyanines (M(Pc)s) featuring a defined metal coordination environment as electrocatalysts for acetylene semihydrogenation. Consequently, CoPc exhibits an ethylene current density of 150.8 mA cm −2 and a ∼ 96% ethylene faradaic efficiency under a pure acetylene stream. In-situ electrochemical Raman and theoretical calculations demonstrate that CoPc favors acetylene absorption/hydrogenation processes. Even for crude ethylene containing 1 × 10 4 ppm acetylene, CoPc manifests a ∼ 99.5% acetylene conversion, a high turnover frequency of 4.86 × 10 –3 s −1 and a large space velocity of 2.4 × 10 5 ml·g cat –1 ·h −1 , outperforming those for reported thermocatalysts. This work facilitates the development of electrocatalytic acetylene semihydrogenation and promises alternatives to traditional thermocatalytic processes.
研究领域:
化学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Materials Au
·
2022
·
IF 0
Qingsong Luo,Hai Wang,Liang Wang,Feng-Shou Xiao
Selective hydrogenation of acetylene to ethylene is an industrially important process to purify the raw ethylene stream for producing high-grade polyethylene. The supported Pd catalyst exhibits superior activity for acetylene hydrogenation but suffers from poor ethylene selectivity because of the easy overhydrogenation to produce ethane. Here, we report that the PdCu alloy nanoparticles within siliceous zeolite crystals effectively tuned Pd-catalyzed overhydrogenation into semihydrogenation. This catalyst displayed an ethylene selectivity of 92.9% with a full conversion of acetylene. Mechanism studies reveal that the zeolite fixation stabilized the alloyed structure, where the electron-enriched Pd surface benefits the rapid ethylene desorption to hinder the deep hydrogenation. This work provides an efficient strategy for a rational design of bimetallic metal catalysts for selective hydrogenations.
研究领域:
催化化学
·
材料科学
·
纳米技术
✓ 已验证
DOI
JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Xiaozhen Shi,Xin Wen,Shilin Nie,Jie Dong,Jingde Li,Yongqing Shi,Huiling Zhang,Guoyi Bai
Nickel is a highly active catalyst for the semi-hydrogenation of alkynes. However, the low selectivity of the alkene product caused by the over-hydrogenation reaction on Ni has hindered its practical applications. In this work, we report a new nickel nitride (Ni 3 N)-catalyzed semi-hydrogenation of alkynes to the corresponding alkenes. The Ni 3 N nanorods were facilely fabricated via a direct pyrolysis of the solid mixture of nickel acetate tetrahydrate and melamine (Mlm). The Ni 3 N phase in the optimum catalyst (Ni 3 N/NC-6/5-550) is shown to be effective and stable in the semi-hydrogenation of alkynes, with a high yield and good selectivity for alkenes ( Z / E ratios up to >99/1). Both terminal and internal alkynes bearing a broad scope of functional groups are readily converted into alkenes with good chemo- and stereoselectivity. Notably, it was found that the over-hydrogenation can be markedly suppressed even at high conversion of alkyne. Density functional theory (DFT) calculations reveal that the low interaction between the alkene product and the Ni 3 N might plays a critical role in the selectivity enhancement.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-9
·
IF 16.6
Bu Jun,Chang Siyu,Li Jinjin,Yang Sanyin,Ma Wenxiu,Liu Zhenpeng,An Siying,Wang Yanan,Li Zhen,Zhang Jian
Alkynols semi-hydrogenation is a critical industrial process as the product, alkenols, have extensive applications in chemistry and life sciences. However, this class of reactions is plagued by the use of high-pressure hydrogen, Pd-based catalysts, and low efficiency of the contemporary thermocatalytic process. Here, we report an electrocatalytic approach for selectively hydrogenating alkynols to alkenols under ambient conditions. For representative 2-methyl-3-butene-2-ol, Cu nanoarrays derived electrochemically from CuO, achieve a high partial current density of 750 mA cm − 2 and specific selectivity of 97% at −0.88 V vs. reversible hydrogen electrode in alkaline solution. Even in a large two-electrode flow electrolyser, the Cu nanoarrays deliver a single-pass alkynol conversion of 93% with continuous production of 2-methyl-3-butene-2-ol at a rate of ~169 g g Cu − 1 h − 1 . Theoretical and in situ electrochemical infrared investigations reveal that the semi-hydrogenation performance is enhanced by exothermic alkynol adsorption and alkenol desorption on the Cu surfaces. Furthermore, this electrocatalytic semi-hydrogenation strategy is shown to be applicable to a variety of alkynol substrates.
研究领域:
化学
·
材料科学
·
催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Xin Song,Fangjun Shao,Zijiang Zhao,Xiaonian Li,Zhongzhe Wei,Jianguo Wang
Precise regulation of reaction selectivity at high conversions is the key to non-terminated alkyne semi-hydrogenation. Herein, a support modification strategy was employed to incorporate trace amounts of Mg elements into alumina support. The modified support loaded Pd catalyst optimized the activity and selectivity of the non-terminated alkyne semi-hydrogenation reaction. The TEM and XRD characterization of the catalysts demonstrated the entry of Mg elements into the Al 2 O 3 lattice to achieve the modification of the support. For the 2-butyne-1-ol semi-hydrogenation reaction, the Pd 0.5 /Mg 1 @Al 2 O 3 catalyst showed 99 % conversion and 97 % selectivity of the cis product at hydrogen pressure of 0.1 MPa and 25 °C. The introduced Mg element changed the electronic structure of Pd nanoparticles in the catalyst. The precise regulation of the 2-butyne-1-ol semi-hydrogenation reaction was achieved by adjusting the ratio of Pd 0 to Pd 2+ using the synergistic effect of Pd 0 and Pd 2+ .
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2013
·Vol. 15
·期 9
·2525-2531
·
IF 6.828
Dongshun Deng,Yang Yang,Yutong Gong,Yi Li,Xuan Xu,Yong Wang
Palladium nanoparticles supported on a mesoporous graphitic carbon nitride, Pd@mpg-C3N4, has been developed as an effective, heterogeneous catalyst for the liquid-phase semihydrogenation of phenylacetylene under mild conditions (303 K, atmospheric H2). A total conversion was achieved with high selectivity of styrene (higher than 94%) within 85 minutes. Moreover, the spent catalyst can be easily recovered by filtration and then reused nine times without apparent lose of selectivity. The generality of Pd@mpg-C3N4 catalyst for partial hydrogenation of alkynes was also checked for terminal and internal alkynes with similar performance. The Pd@mpg-C3N4 catalyst was proven to be of industrial interest.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Xin Song,Wenjie Pan,Fangjun Shao,Zijiang Zhao,Xiaonian Li,Zhongzhe Wei,Jianguo Wang
The development of alkyne semihydrogenation catalysts with high conversion and selectivity under mild conditions is extremely challenging. Here, the modulation of Pd by different crystalline aluminas was investigated to improve the reaction performance. XPS confirmed that different crystalline aluminas modified the electronic structure of palladium. The Pd0.5/γ-Al2O3 catalyst with a Pd loading of 0.48 wt % attained 98% conversion and 91% selectivity. Stronger interaction of the γ-Al2O3 support with the loaded Pd nanoparticles resulted in electron deflection toward the support. The electronic structure of Pd was altered by modulating the crystallographic shape of the support, resulting in metal nanoparticles containing more Pd2+. Electron-deficient Pd2+ adsorbs more strongly on an electron-rich C≡C, which in turn modulates the competitive adsorption of alkenes and alkynes. Finally, the effective semihydrogenation of phenylacetylene was realized at low temperature and pressure.
研究领域:
化学工程
·
催化
·
材料科学
✓ 已验证
DOI
高影响因子
AICHE JOURNAL
·
2025
·
IF 4
Ziqi Bian,Minhao Chen,Xiaohu Ge,Ningchao Zhu,Yueqiang Cao,Hao Jiang,Jing Zhang,Gang Qian,Xinggui Zhou,Xuezhi Duan
Designing and fabricating uniformly dispersed non-precious metal active sites with tuned geometric configurations and local coordination environments for the selective conversion of functional groups to desired products is of great importance but remains challenging in industrial catalytic processes. In this work, we propose a straightforward method for synthesizing the Co 3 Sn 2 intermetallic catalyst through the structural conversion of layered double hydroxide precursors, thereby constructing suitable Sn-modified Co active sites and an optimized catalytic environment for propyne semihydrogenation. Characterizations using x-ray diffraction, high-resolution transmission electron microscopy, and x-ray absorption spectroscopy characterizations are combined to identify the formation of P6 3 /mmc Co 3 Sn 2 intermetallic phase. Catalytic performance tests show that the Co 3 Sn 2 catalyst achieves 95.0% propylene selectivity with nearly complete propyne conversion. Temperature-programmed surface reaction and desorption measurements combined with theoretical calculations demonstrate that the good selectivity is driven by the facile desorption of propylene from Sn-modified Co sites rather than its further hydrogenation.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）