Plasmonic photocatalysis is promising for solar-driven chemical transformations under mild conditions; however, conventional materials like aluminum, copper, silver, and gold are resonant at short wavelengths, limiting their use in the red to near-infrared sunlight spectrum. In this study, we have developed a class of antenna-reactor (AR) photocatalyst based on two-dimensional (2D) plasmonic materials, Ti3C2Tx, also known as MXenes. A Ru-loaded Ti3C2Tx plasmonic photocatalyst achieves a turnover frequency of approximately 2 s–1 and energy efficiency of 10% for hydrogen production under 660 nm light excitation, being 2–3 orders of magnitude superior to the performance achieved in thermocatalysis. This 2D plasmonic antenna demonstrates superiority over the benchmark CuRu surface-alloy AR structure in hot-electron-driven processes under red light excitation. Kinetic studies suggest that the rate-determining step in both photo- and thermocatalysis is nitrogen’s associative desorption. Hot electrons enhance activity by promoting the removal of adsorbed nitrogenous species.
Wang Juping,Zhu Fengfan,Qin Yu,Zhu Yuan-Hao,Zhou Jiancheng,Li Naixu
This research is centered on the design and synthesis of a highly efficient heterogeneous catalyst, 1%Ru-MgO- 400 °C, for the hydrogenation of pyrrole to pyrrolidine. As a key intermediate in pharmaceutical manufacturing and fine chemical production, pyrrolidine synthesis poses significant challenges in terms of efficiency. In this work, MgO was synthesized via the calcination of Mg(OH) 2 , followed by the deposition of Ru onto MgO- 400 °C through a sodium borohydride reduction approach to produce the 1%Ru-MgO- 400 °C catalyst. The catalyst demonstrated exceptional performance under conditions of 170 °C and 3.5 MPa H 2 pressure, achieving complete conversion of pyrrole and a 100% yield of pyrrolidine. Advanced characterization methods such as XRD, TG, BET, SEM and HR-TEM were used to analyze the catalyst, revealing that the ruthenium nanoparticles were uniformly loaded on the MgO carrier to form a highly dispersed active site, while the crystal structure of MgO remained intact with excellent thermal stability, providing a structural basis for the efficient performance of the catalyst. Additionally, the catalyst exhibited remarkable stability and retained high activity over multiple reaction cycles, highlighting its suitability for industrial-scale applications. The findings of this study contribute novel perspectives to the development of robust and efficient hydrogenation catalysts and present a sustainable approach for the environmentally friendly synthesis of pyrrolidine. Graphic
Lei CHEN,Yu ZHANG,Bin SUN,Juan HE,Shuai KANG,Zhong-Qiu HUA,Chen TIAN
The production of a large number of metal oxide semiconductor materials is more for design needs, while theoretical exploration is relatively less concerned. In this work, WO 3 nanoparticles were prepared by the tungstic acid thermolysis method, and the catalysts of Pt and Ru were loaded on the surface of nanoparticles with a wet impregnation method. As expected, the sensitive responses were enhanced significantly with the additional loading of Pt, which revealed that bimetallic loading could achieve better properties with a smaller loaded amount than single metal. According to the power-law response to oxygen and H 2 -TPR results, the sensitization mechanism of noble metals loaded WO 3 to acetone as the typical VOCs was investigated. The results showed that the sensing processes were dominated by oxygen adsorption behavior and there was no difference with the loading of Ru. Furthermore, the power-law coefficient n became smaller with Pt loading. It is proposed that oxygen adsorbates on the surface become more active due to Pt. We would like to propose further a perspective, i.e., polymetallic loading that utilizes the properties of different metals to achieve synergism.
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