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Synergism of Ultrasmall Pt Clusters and Basic La2O2CO3 Supports Boosts the Reverse Water Gas Reaction Efficiency
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-01-20 , DOI: 10.1002/aenm.202203806
Rui Zhang 1, 2 , Xiao Wang 1, 2 , Ke Wang 1, 2 , Huilin Wang 1, 2 , Li Liu 1, 2 , Xueting Wu 1, 2 , Baokang Geng 1, 2 , Xiang Chu 1, 2 , Shuyan Song 1, 2 , Hongjie Zhang 1, 2, 3
Affiliation  

The reverse water-gas shift reaction (RWGS) has been regarded as a promising approach for fighting climate change caused by the excessive emission of the greenhouse gas CO2, but it still suffers from relatively poor low-temperature reactivity. Herein, a high-performance RWGS catalyst composed of ultrasmall Pt clusters (1.38 nm on average) anchored by La2O2CO3 support (PtNC/LOC), which possesses a record CO production rate of 2678 molCO molPt−1 h−1 with nearly 100% CO selectivity at 300 °C, is reported. The specific activity is nearly 1.5 and 7.9 fold higher than that of Pt single atoms and nanoparticles on La2O2CO3, respectively. More importantly, over 87.7% of the initial activity of PtNC/LOC remains after 80 h constant operation at 380 °C, firmly verifying the structural robustness. LOC support is essential, because of not only the moderate basicity that can boost the reaction efficiency but also the strong interaction with Pt species that can stabilize the ultrasmall particle size. Further investigations also point out the key role of the Pt clusters. The two key steps, CO2 adsorption, and CO desorption, individually prefer electron-rich and electron-deficient Pt species. Ultrasmall Pt clusters successfully integrate the unique surface states of single atoms and nanoparticles, thus achieving excellent low-temperature RWGS performance.

中文翻译:

超小 Pt 团簇与碱性 La2O2CO3 载体的协同作用提高了逆水气反应效率

逆向水煤气变换反应(RWGS)被认为是应对因温室气体CO 2过度排放引起的气候变化的一种有前途的方法,但它仍然存在低温反应性相对较差的问题。在此,由 La 2 O 2 CO 3载体锚定的超小 Pt 团簇(平均 1.38 nm)组成的高性能 RWGS 催化剂(Pt NC /LOC),其 CO 产率达到创纪录的 2678 mol CO mol Pt -1据报道,h -1在 300 °C 下具有接近 100% 的 CO 选择性。比活度比 La 上的 Pt 单原子和纳米粒子高近 1.5 和 7.9 倍2 O 2 CO 3,分别。更重要的是,在 380 °C 下持续运行 80 小时后, Pt NC /LOC初始活性的 87.7% 以上仍然存在,有力地验证了结构的稳健性。LOC 支持是必不可少的,因为不仅因为适度的碱度可以提高反应效率,还因为与 Pt 物质的强相互作用可以稳定超小粒径。进一步的调查还指出了 Pt 簇的关键作用。两个关键步骤,CO 2吸附和 CO2 解吸分别偏好富电子和缺电子的 Pt 物种。超小型 Pt 团簇成功整合了单原子和纳米粒子的独特表面态,从而实现了优异的低温 RWGS 性能。
更新日期:2023-01-20
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