Photothermal Conversion of Biopolyols and Sugars into Syngas over Pd–PdO/TiO2

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL
Jingxuan Yang, Hongru Zhou, Jincheng Luo, Min Wang
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引用次数: 0

Abstract

Photocatalysis is promising for reforming biopolyols and sugars into syngas (CO+H2), while the carbon is easily overoxidized to CO2 due to the hydroxyl radical (•OH) under aqueous conditions. Targeting this problem, a temperature-controlled photo-reforming strategy is proposed and the Pd–PdO/TiO2 is used as the catalyst. The photocatalytic reforming process effectively breaks the C–H and C–C bonds of biomass to produce radicals. The increased reaction temperature not only increases the photocatalytic reaction rate but also thermodynamically fine-tunes the radical reaction process, facilitating the decarbonylation of acyl radical intermediates and prohibiting its overoxidation to CO2. With the reaction temperature increased from 40 to 180 °C, the CO selectivity from glycerol reforming over Pd–PdO/TiO2 catalyst under aqueous conditions improves significantly from 1.6% to 66%. The unique Pd–PdO/TiO2 structure plays an important role in syngas production. On one hand, the decorated Pd species significantly promote light adsorption and the separation of photogenerated charge carriers. On the other hand, the PdO nanoparticles effectively facilitate the adsorption and decarbonylation process of acyl radical intermediates. A CO yield of over 60% for glycerol reforming under photothermal conditions can be obtained over Pd–PdO/TiO2, which is 3 times that of pristine TiO2 (20%). A wide range of biopolyols and sugars can also be converted into syngas through this photothermal system with a CO yield of 20–66%, along with 0.17–2.13 mmol·g–1·h–1 H2 evolution.

Abstract Image

生物多元醇和糖在Pd-PdO /TiO2上光热转化为合成气
光催化在将生物多元醇和糖转化为合成气(CO+H2)方面很有前景,而在水条件下,由于羟基自由基(•OH)的存在,碳很容易被过度氧化为二氧化碳。针对这一问题,提出了一种以Pd-PdO /TiO2为催化剂的温控光重整策略。光催化重整过程有效地破坏了生物质的C-H和C-C键,产生自由基。升高的反应温度不仅提高了光催化反应速率,而且对自由基反应过程进行了热力学微调,促进了酰基自由基中间体的脱碳,防止其过度氧化为CO2。当反应温度从40℃提高到180℃时,水溶液条件下Pd-PdO /TiO2催化剂上甘油重整CO的选择性从1.6%提高到66%。独特的Pd-PdO /TiO2结构在合成气生产中起着重要作用。一方面,修饰后的钯显著促进了光吸附和光生载流子的分离。另一方面,PdO纳米颗粒有效地促进了酰基自由基中间体的吸附和脱碳过程。Pd-PdO /TiO2在光热条件下重整甘油的CO产率可达60%以上,是原始TiO2(20%)的3倍。广泛的生物多元醇和糖也可以通过该光热系统转化为合成气,CO产率为20-66%,氢气的析出率为0.17-2.13 mmol·g-1·h-1。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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