Selective Hydrogenation of Acetylene to Ethylene over the Surface of Sub-2 nm Pd Nanoparticles in Miscanthus sinensis-Derived Microporous Carbon Tubes

Abstract

As one of the organic carbon-rich feedstocks, Miscanthus sinensis is an interesting candidate for producing many high-value materials and chemicals. In this study, M. sinensis -derived activated carbon (msAC) particles with ca. 3.4 nm average pore size have been prepared by a simple carbonation method for supporting Pd nanoparticles (NPs) to hydrogenate acetylene. Catalytic test results showed that the 0.25% Pd/msAC catalyst could convert ∼99.9% of acetylene with ∼99.9% of ethylene selectivity. The life test result strongly demonstrated that the catalyst had a good durability for long-term (>100 h) acetylene hydrogenation with high conversion (∼99.9%) and ethylene selectivity (∼93.1%) at 260 °C with a space velocity of 80,000 h–1. The characterization results indicated that the msAC with the micro- and nanoscale pore structure and uniformly distributed oxygen-containing functional groups could efficiently disperse Pd nanoparticles and promote their Pd (111) crystal plane exposure. The above structure nature was co-contributing to the catalyst to choose the energetically favorable path for efficient acetylene hydrogenation and ethylene desorption. This work opens up valuable insights into the high-value utilization of M. sinensis biomass to design an efficient isolated Pd NP catalyst.

Facile Synthesis of Palladium‐Silver Dilute Alloy Catalyst for Acetylene Hydrogenation

“…Very recently, the dilute alloys [4] including single‐atom alloy (SAA) or dimer alloy (DA) have attracted great attention, because they are usually active and robust for various kinds of catalysis reactions. In addition, the well‐defined nature of the active centers in the dilute alloys makes them viable to perform unambiguous study modeling.…”

Effective Inhibition of Ethane Generation on Fe5C2 Nanoparticles Doped with ppm Level of Pd for Selective Hydrogenation of Acetylene

“…Ethylene is a key industrial chemical mainly derived from thermal cracking of hydrocarbons. − The cracked gas usually contains traces of acetylene which can deactivate the catalyst for downstream ethylene polymerization. − At the same time, acetylene will also cause quality degradation of polyethylene . Selective hydrogenation is the most economical and convenient way to handle the acetylene impurity in cracked gas, and has always attracted the attention of many researchers. , Meanwhile, acetylene hydrogenation is still a study of great potential application value in producing ethylene in countries where oil is scarce but rich in coal resources. , It can alleviate the dependence of these countries on crude oil to a large extent. In the process of acetylene semihydrogenation, preventing the intermediate product ethylene from being further hydrogenated to ethane has always been the crucial topic.…”

“…8 Selective hydrogenation is the most economical and convenient way to handle the acetylene impurity in cracked gas, and has always attracted the attention of many researchers. 9,10 Meanwhile, acetylene hydrogenation is still a study of great potential application value in producing ethylene in countries where oil is scarce but rich in coal resources. 11,12 It can alleviate the dependence of these countries on crude oil to a large extent.…”

Metallic Iron Nanocatalysts for the Selective Acetylene Hydrogenation under Industrial Front-End Conditions

“…40,41 Various results can be optimized 42,43 through nanoparticle size, 44,45 morphology, 46−48 surface modification of organic ligands, 48−50 and support-based interactions. 51,52 Most recent deployments on acetylene hydrogenation include Pt−Sn bimetallic nanoparticles confined in mesoporous silica walls, 53 Pd on fiberglass 54 or in microporous carbon tubes, 55 gold nanoparticles supported on Ce−Zr oxides, 38 Cu 2 O nanocubes, 56 and many more. The preparation of iron nanoparticles has especially led to vast improvements in activity and selectivity for many different reactions.…”

“…Another approach under investigation is the further optimization of more abundantly available alternatives such as nickel, − copper, ,, and gold − as catalysts for selective acetylene hydrogenation in order to compete with the palladium-based catalysts. Over the last decades nanoparticles have been the focus of both approaches and many studies in general. , Various results can be optimized , through nanoparticle size, , morphology, − surface modification of organic ligands, − and support-based interactions. , Most recent deployments on acetylene hydrogenation include Pt–Sn bimetallic nanoparticles confined in mesoporous silica walls, Pd on fiberglass or in microporous carbon tubes, gold nanoparticles supported on Ce–Zr oxides, Cu 2 O nanocubes, and many more. The preparation of iron nanoparticles has especially led to vast improvements in activity and selectivity for many different reactions. − For the selective acetylene hydrogenation iron nanoparticles have been deployed as a coating for nanocatalysts, embedded in metal organic frameworks and in inter- and bimetallic nanocatalysts.…”