Carbon Monoxide Tolerant Pt-Based Electrocatalysts for H2-PEMFC Applications: Current Progress and Challenges
Abstract
:1. Introduction
2. Fundamentals of CO Tolerance
2.1. HOR and CO Poisoning Kinetics
2.2. CO Tolerance Mechanisms
- The adsorbate orbitals are hybridized with the s-state of Pt. This interaction results in the energy downshifting and broadening of both 2π* and 5σ CO states, as shown in Figure 2a. Schiros et al. [42] suggested that this type of hybridization positively polarizes the metal s-state due to an electron distribution (Figure 2a(i)); therefore, the orbital of the adsorbate is coordinated through an attractive electrostatic interaction, promoting to some extent the bond formation;
- Two stabilization effects occur synergistically between the renormalized CO states and Pt d-state. Through this interaction, the respective bonding and antibonding states of 5σ and 2π* states are formed. The contribution of the 5σ antibonding state is considered minimal. First, an electron transfer arises from the highest occupied molecular orbital (HOMO) of CO, the filled 5σ bonding state, to the Pt d-state, increasing its electron density. To compensate for this effect, electrons are back-donated from the Pt d-state to the lowest occupied molecular orbital (LUMO) of CO, the empty 2π* antibonding state (Figure 2a(ii)); therefore, total charge stabilization between the interacted DOS is achieved, leading to the Pt-CO binding [43,44,45].
2.3. Energetic View of CO Tolerance
3. Overview of State-of-the-Art CO-Tolerant Electrocatalysts
3.1. Pt-Based Electrocatalysts Supported on Carbon
3.1.1. Alloys
3.1.2. Core–Shell Structures
3.1.3. Combinations with Metal Oxides
3.1.4. Surface-Modified Pt/C
3.2. Pt-Based Electrocatalysts Supported on Alternative Materials
3.2.1. Advanced Carbonaceous Supports
3.2.2. Transition Metal Oxides and Carbides
4. Outlook
5. Concluding Remarks
- The optimal regulation of the alloying degree of Pt alloys via appropriate synthesis pathways can considerably improve CO tolerance and stability; however, since the added non-noble metals are exposed on the catalyst surface in the alloyed structures, Pt alloys do not generally present adequate stability for practical utilization. Nevertheless, examination of the Pt alloys is essential to reveal the correlations between the physicochemical properties, stability, and CO tolerance mechanisms;
- The combination of Pt-based electrocatalysts with TMOs can enhance the CO tolerance through the promotion of the bifunctional mechanism via the oxygenated species on their surfaces; however, to avoid the blockage of the Pt’s active surface and the dissolution of metal oxides, the structure of the developed electrocatalysts should be suitably controlled;
- The surface-sensitive nature of CO electrooxidation enables the enhancement of the CO tolerance of Pt/C (susceptible to CO poisoning) by controlling its morphology and structure through suitable synthesis routes. The regulation of the lattice strain, electronic structure, metal NP size, terraces adlayers, surface defects, and exposed crystalline facets can positively affect the CO adsorption and CO oxidation;
- The substitution of conventional the carbon black support with advanced carbonaceous materials can improve the CO tolerance through better electronic interactions between the deposited metal NPs and the support. Additionally, the functionalization of the carbon surface via chemical pre-treatment or doping with elements promotes the bifunctional mechanism, accelerating CO oxidation;
- The utilization of Mo and W oxides and carbides as alternative catalyst supports can help avoid the use of the corrosive carbon and enhance CO tolerance, mainly through the bifunctional characteristics of Mo and W; however, to ensure adequate stability, Mo and W atoms must be incorporated sufficiently in the composite;
- Core–shell-structured CO-tolerant electrocatalysts are the most promising for practical applications. Generally, the encapsulation of non-noble-metal-based core within the Pt shell prevents its leaching, resulting in excellent stability improvements. Concurrently, through the electronic modification introduced by the core to the Pt shell, the CO adsorption is significantly suppressed. Novel approaches related to 2D material shells, such as the use of hexagonal boron nitride, present exceptional potential for further research. Similar behavior can be obtained with 2D material shells by modifying the surfaces of conventional electrocatalysts with organic compounds.
Author Contributions
Funding
Acknowledgments
Conflicts of Interest
References
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Electrocatalyst | Experimental Conditions | Refs (Data) | Electrocatalyst | Experimental Conditions | Refs (Data) |
---|---|---|---|---|---|
PtRu@h-BN/C | 25 °C, 0.1 M HClO4, 20 mV/s | [95] (1) | WO3/Ptpc | 25 °C, 0.1 M HClO4, 50 mV/s | [136] (18) |
PtxAL‒Pt69Co31/C | 70 °C, 0.1 M HClO4, 20 mV/s | [100] (2) | Pt-BeO/C | 25 °C, 0.1 M HClO4, 20 mV/s | [137] (19) |
Pt2AL −PtFe/C | 70 °C, 0.1 M HClO4, 20 mV/s | [99] (3) | Pt/C+WOx | 25 °C, 0.5 M HClO4, 100 mV/s | [138] (20) |
Pt2AL −PtCo/C | 70 °C, 0.1 M HClO4, 20 mV/s | [99] (4) | Pt/C-RuOxHy_ | 25 °C, 0.5 M H2SO4, 20 mV/s | [139] (21) |
Pt2AL −PtNi/C | 70 °C, 0.1 M HClO4, 20 mV/s | [99] (5) | Pt/C/WO3 | 25 °C, 0.1 M H2SO4, 10 mV/s | [106] (22) |
Pt/TiWN/C | 25 °C, 0.1 M HClO4, 50 mV/s | [140] (6) | PtRuNi/C | 25 °C, 0.5 M H2SO4, 10 mV/s | [94] (23) |
Pt/TiWC/C | 25 °C, 0.1 M HClO4, 50 mV/s | [140] (7) | Pt/Ru0.7Ti0.3O2 | 25 °C, 0.1 M HClO4, 20 mV/s | [141] (24) |
Ru(ns)-PtRu/C | 25 °C, 0.1 M HClO4, 10 mV/s | [105] (8) | Pt-HxMoO3 | 25 °C, 0.5 M H2SO4, 2 mV/s | [142](25) |
RuO2.1ns-PtRu/C | 25 °C, 0.1 M HClO4, 10 mV/s | [105] (9) | Pt2Ru3/Sb-SnO2 | 70 °C, 0.1 M HClO4, 20 mV/s | [143] (26) |
[email protected](ns)/C | 25 °C, 0.1 M HClO4, 10 mV/s | [144] (10) | PtRu/WxCyOz | 25 °C, 0.5 M HClO4, 100 mV/s | [128] (27) |
Pt@h-BN/C | 25 °C, 0.1 M HClO4, 20 mV/s | [96] (11) | Pt/PEI-hex-WO3 | 25 °C, 0.5 M H2SO4, 20 mV/s | [131] (28) |
Pt-Ru-Sn/C | 60 °C, 0.06 M HClO4, 10 mV/s | [77] (12) | Pt/Ti0.7W0.3O2-C | 25 °C, 0.5 M H2SO4, 10 mV/s | [145] (29) |
Ru@Pt/C | 25 °C, 0.5 M H2SO4, 10 mV/s | [146] (13) | Pt/Ti0.7Mo0.3O2-C | 25 °C, 0.5 M H2SO4, 10 mV/s | [145] (30) |
Pt/C MFP90° | 25 °C, 0.5 M H2SO4, 10 mV/s | [109] (14) | Ru@Pt/C-TiO2 | 25 °C, 0.5 M H2SO4, 10 mV/s | [147] (31) |
Pt/ITO/CB | 25 °C, 0.1 M HClO4, 20 mV/s | [148] (15) | Pt/Ti0.6Mo0.4O2-C | 25 °C, 0.5 M H2SO4, 10 mV/s | [130] (32) |
PtRu/SnO2/C | 60 °C, 0.1 M HClO4, 10 mV/s | [104] (16) | Pt/N-GNP | 25 °C, 0.5 M H2SO4, 10 mV/s | [122] (33) |
RuO2(ns)/Pt | 25 °C, 0.1 M HClO4, 50 mV/s | [149] (17) | Pt/TiO2NCs-C | 25 °C, 0.5 M H2SO4, 50 mV/s | [150] (34) |
Electrocatalyst | Advantages | Challenges | Refs |
---|---|---|---|
PtRuNi/C (composition gradient shell) | - Only 11% performance decay after 10 ppm CO poisoning - Complete stability after 100 h of operation for 10 ppm CO/H2 feed | - Unknown CO tolerance under poisoning with greater than 10 ppm CO concentrations - Complicated synthesis method | [94] |
PtxAL-Pt69Co31/C | - 95% HOR activity retention after 1000 ppm CO poisoning at 70 °C - 78% HOR activity retention after 1000 ppm CO poisoning and after a durability test of 4000 cycles | - Unknown CO tolerance behavior under practical H2-PEMFC operation | [100] |
PtRu@h-BN/C | - Only 18 and 26 mV potential loss at 0.2 and 0.6 A cm−2, respectively, after 30 ppm CO + 25% CO2 poisoning - Thermochemically and electrochemically stable | - Unknown stability for long-term H2-PEMFC operation under CO poisoning - Complicated synthesis method | [95] |
Pt/TixMo1-xO2-C (x = 0.8–0.6) | - CO oxidation at potentials smaller than 250 mV - 130 mV overpotential at 1 A cm−2 after 100 ppm CO poisoning | - Lower HOR activity in the absence of CO than Pt/C, due to lower support conductivity - Inadequate stability due to dissolution of non-incorporated Mo | [129,130,145] |
Pt/C MFP90° | - Only 12% loss in maximum power density after 100 ppm CO poisoning | - High PGM loading | [109] |
Pt/C coated with DAcPy | - 87% HOR activity retention after 5 h of continuous poisoning with 100 ppm CO | - High PGM loading - Unknown CO tolerance behavior under practical H2-PEMFC operation | [110] |
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Molochas, C.; Tsiakaras, P. Carbon Monoxide Tolerant Pt-Based Electrocatalysts for H2-PEMFC Applications: Current Progress and Challenges. Catalysts 2021, 11, 1127. https://doi.org/10.3390/catal11091127
Molochas C, Tsiakaras P. Carbon Monoxide Tolerant Pt-Based Electrocatalysts for H2-PEMFC Applications: Current Progress and Challenges. Catalysts. 2021; 11(9):1127. https://doi.org/10.3390/catal11091127
Chicago/Turabian StyleMolochas, Costas, and Panagiotis Tsiakaras. 2021. "Carbon Monoxide Tolerant Pt-Based Electrocatalysts for H2-PEMFC Applications: Current Progress and Challenges" Catalysts 11, no. 9: 1127. https://doi.org/10.3390/catal11091127