Synthetic Strategies of Supported Pd-Based Bimetallic Catalysts for Selective Semi-Hydrogenation of Acetylene: A Review and Perspectives
Abstract
:1. Introduction
2. Synthesis of Supported Pd-Based Bimetallic Nano-Catalysts
2.1. Wet Chemistry Technique
2.1.1. Incipient Wetness Impregnation (IWI) Method
2.1.2. Precipitation Method
2.1.3. Sol-Gel Method
2.1.4. One-Pot Reduction Deposition (One-Pot RD) Method
2.1.5. Sequential Reduction-Deposition Method (S-RD)
2.1.6. Photochemical Reduction (PR)
2.1.7. Colloidal Synthesis
2.1.8. Hydrothermal/Solvothermal Method
2.1.9. Surface Inorganometallic Chemistry
2.2. Plasma Treatment
2.3. Thermal Pyrolysis
2.4. Vapor Deposition and Electrochemical Deposition
2.5. Ball Milling
3. Synthesis of Single Atom Alloy and Bimetallic Dual Atom Catalysts
4. Conclusions
- In summary, the synthesis of supported Pd-based bimetallic catalysts for selective semi-hydrogenation of acetylene is possible by a variety of fabrication procedures. However, it also needs to be aware that each synthesis method has its own characteristics, whether it is old or new; different methods have different application conditions and may be applicable to different catalyst systems. In order to establish a clear comparison of different synthesis strategies, their key characteristics, advantages, and disadvantages, and the catalyst systems that they have been applied to, are listed in Table 1.
- 2.
- The continuous improvement of the methods and their use in appropriate combinations will continue to be a research focus, contributing to the further improvement of the palladium-based bimetallic catalyst performance.
- 3.
- In any case, however, the ultimate application of palladium-based bimetallic catalysts for the selective semi-hydrogenation of acetylene is an industrial-scale reaction scenario. Therefore, to develop more simple and efficient catalyst preparation methods to meet the requirements of industrial-scale reactions will be one of the goals that researchers are constantly striving for.
- 4.
- The development of preparation methods with the participation of environmentally benign visible or ultraviolet (UV) light, cold plasma, and other new energy sources should be a development direction.
- 5.
- Dual-atom catalysts (DACs) theoretically can achieve the same high loadings as nano-catalysts and, at the same time, can achieve the same mono-dispersion of active metal atoms as single-atom alloy catalysts. With that in mind, supported Pd-based dual-atom catalysts should be the most promising alternative for selective semi-hydrogenation of acetylene in the future.
- 6.
- Most recently, machine learning (ML), combining experiments, has brought new solutions for the screening of active metals and suitable supports and for the performance optimization of catalyst systems [43,185]. The Liu group [43,185] performed pioneering works for the design of supported PdAg bimetallic catalysts for the acetylene semi-hydrogenation reaction. Reaction test results indicated a new record for the low-temperature selective semi-hydrogenation of acetylene: 97.2% selectivity and 100% acetylene conversion below 100 °C; moreover, the resulting Pd1Ag3/r-TiO2 is rather stable, above 95% selectivity at the high conversion (>98%) over a 120 h experiment. Thus, it could be reasonable to speculate that emerging science such as artificial intelligence (AI), machine learning (ML), big data, and supercomputing combined experiments demonstrate a broad prospect for the rational and efficient design of complex heterogeneous catalytic systems.
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Synthetic Method | Key Features | Synthesized Catalyst Types | Merits | Demerits | Example and Ref. |
---|---|---|---|---|---|
Incipient wetness impregnation (IWI) method | Most widely used preparation method | Supported bimetallic nano-catalysts/single atom alloy | Easy operation; low cost; high production capacity; sample resistance to sintering; SMSI | Minimal control of particle size and element distribution; calcination contamination | Pd1Ag3/r-TiO2 (T750) [185] |
Co-precipitation (CP) | Simultaneous precipitation of the two metals and the support | Supported bimetallic nano-catalysts | Easy control of particle size and element distribution; maximum metal loading and metal-support interaction | Accurate control of synthesis conditions; impurity (by precipitant) removal is required; small proportion of active components on the surface; thermal treatment | Mco-PdCu/MgAl-cHT [75] |
Deposition-precipitation (DP) | Widely used in the preparation of supported metal catalysts; one-pot synthesis | Supported bimetallic nano-catalysts/single atom alloy/bimetallic dual atom catalysts | Particle size and component distribution are generally superior to those prepared by IWI; SMSI | Accurate control of synthesis conditions; impurity removal is required; metal-support interaction is required; thermal treatment; easy liquid-phase nucleation | Pd1Cu1/ND@G (DACs) [41] |
One-pot reduction deposition (one-pot RD) | One-pot synthesis; simultaneous reduction of the two metals to deposit on the support; chemical reducing agents participate in the reduction. | Supported bimetallic nano-catalysts | Particle size and component distribution are generally superior to those prepared by DP | Accurate control of synthesis conditions; impurity removal is required; metal-support interaction is required; thermal treatment; existing liquid-phase nucleation and mono-metal deposition | PdBi/Calcite [81] |
Electroless reduction deposition (eless-RD) | Parent metal activates chemical reducing agents to reduce the secondary metal; atom-by-atom deposition on the parent metal | Supported bimetallic nano-catalysts | Available complex structures, e.g., core–shell structures; achieving deposition of the dopant metal that cannot be performed by GR | No deposition on the support is still a question to consider; in most of cases, more precise control of synthesis parameters than GR | Cu–Pd/TiO2 [99] |
Galvanic replacement (GR) | Supported parent metal is prepared first; atom-by-atom metal exchange driven by reduction potential. | Supported bimetallic nano–catalysts/single atom alloy | Available special compositions and structures; shape of the template maintained | Complicated steps; deposition depends on the difference in reduction potentials between the two metals | Pd–Ag/SiO2 [101] |
Controlled surface reaction (CSR) | Reduction of the parent metal occurs first; strict operation conditions | Supported bimetallic nano-catalysts/single atom alloy | Available complex structures | High-level complex steps; need to perform in an inert atmosphere and anhydrous solutions | CuPd0.02/TiO2 [97] |
Photochemical reduction (PR) | Greenness; visible or ultraviolet (UV) light drives reactions | Supported bimetallic nano-catalysts/single atom alloy/bimetallic dual atom catalysts | Simplicity; high efficiency; greenness; normally room temperature and atmospheric pressure | Some metal atoms do not sensitively respond to irradiation | Pd9Au1/ZnTi [112] |
Colloidal synthesis | Metal precursors form a metallic colloid to support on the matrix | Supported bimetallic nano-catalysts/single atom alloy | Easy and flexible control of particle shape, size, and element distribution | Precise control of synthesis conditions and impurity removal is generally required | Au@Pd/TiO2 [119] |
Sol-gel method | The precursors undergo the processes of hydrolysis and polymerization, forming sol and then gel | Supported bimetallic nano-catalysts/single atom alloy | Easy control of particle size and element distribution at the atomic level; facile synthesis condition | High price of metal precursors; environmental health issues; long-time synthesis. | CuPd/ZIF-8 [79] |
Physical vapor deposition (PVD) | Physical vaporization of metals; model catalyst preparation; layer-by-layer deposition on the matrix | Supported bimetallic nano-catalysts/single atom alloy | Simple steps; environmental friendliness; diverse coating material availability; controllable size and dispersion | High equipment cost; high process temperature; high surface cleanliness; UHV conditions; not suitable for deposition on a complex surface | GaPd2/Si(111) [159] |
Atomic layer deposition (ALD) | Atomic layer-by-layer deposition; ordered self-terminated reduction occurs on the substrate surface; gaseous metal molecule precursor | Supported bimetallic nano-catalysts/single atom alloy | Atomically distributed; flexible control of the surface, composition, overlayers, and even atomic level thickness; extraordinary reproducibility | High equipment cost; high price of metal precursors; UHV conditions; slow ALD progression | Ga2O3-coated Pd@Ag/SiO2 [160] |
Electrochemical deposition (ECD) | Reactions are driven by an outside current basis | Supported bimetallic nano-catalysts/single atom alloy | Near ambient conditions; efficient usedness of precursors; easy fabrication with excellent control of the morphology and composition with high reproducibility; inexpensive method | Need a sophisticated instrument; poor scalability | Cu dendrites [8] |
Cold plasmas treatment | A partially ionized gas containing many highly active species; non-equilibrium state | Supported bimetallic nano-catalysts | A more efficient, controlled, and mild method, compared with the traditional thermal methods | Specialized equipment | Au–Ag/SiO2 [135] |
Thermal pyrolysis | Thermal pyrolysis and carbonization of organic or polymer materials and metals with van der Waals force or chemical bonding force | Supported bimetallic nano-catalysts/single atom alloy/bimetallic dual atom catalysts | Simplicity; simultaneous one-step preparation of support and active metal | Long reaction time; not easy to control particle size and element distribution; excessive energy usage; air contamination | Pd–Zn-ins/CNS [153] |
Ball milling | The simplest and most efficient mechanical process | Supported bimetallic nano-catalysts/single atom alloy | Extensive range of applications; simplicity; safety | Specialized heavy equipment is required; big power loss; contamination and noise | Pd–Ag/α-Al2O3 [2] |
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Cao, X.; Jang, B.W.-L.; Hu, J.; Wang, L.; Zhang, S. Synthetic Strategies of Supported Pd-Based Bimetallic Catalysts for Selective Semi-Hydrogenation of Acetylene: A Review and Perspectives. Molecules 2023, 28, 2572. https://doi.org/10.3390/molecules28062572
Cao X, Jang BW-L, Hu J, Wang L, Zhang S. Synthetic Strategies of Supported Pd-Based Bimetallic Catalysts for Selective Semi-Hydrogenation of Acetylene: A Review and Perspectives. Molecules. 2023; 28(6):2572. https://doi.org/10.3390/molecules28062572
Chicago/Turabian StyleCao, Xinxiang, Ben W.-L. Jang, Jiaxue Hu, Lei Wang, and Siqi Zhang. 2023. "Synthetic Strategies of Supported Pd-Based Bimetallic Catalysts for Selective Semi-Hydrogenation of Acetylene: A Review and Perspectives" Molecules 28, no. 6: 2572. https://doi.org/10.3390/molecules28062572