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1.
Angew Chem Int Ed Engl ; : e202409001, 2024 Jul 11.
Article in English | MEDLINE | ID: mdl-38990826

ABSTRACT

Formic acid (FA) dehydrogenation and CO2 hydrogenation to FA/formate represent promising methodologies for the efficient and clean storage and release of hydrogen, forming a CO2-neutral energy cycle. Here, we report the synthesis of highly dispersed and stable bimetallic Pd-based nanoparticles, immobilized on self-pillared silicalite-1 (SP-S-1) zeolite nanosheets using an incipient wetness co-impregnation technique. Owing to the highly accessible active sites, effective mass transfer, exceptional hydrophilicity, and the synergistic effect of the bimetallic species, the optimized PdCe0.2/SP-S-1 catalyst demonstrated unparalleled catalytic performance in both FA dehydrogenation and CO2 hydrogenation to formate. Remarkably, it achieved a hydrogen generation rate of 5974 molH2 molPd-1 h-1 and a formate production rate of 536 molformate molPd-1 h-1 at 50 °C, surpassing most previously reported heterogeneous catalysts under similar conditions. Density functional theory calculations reveal that the interfacial effect between Pd and cerium oxide clusters substantially reduces the activation barriers for both reactions, thereby increasing the catalytic performance. Our research not only showcases a compelling application of zeolite nanosheet-supported bimetallic nanocatalysts in CO2-mediated hydrogen storage and release but also contributes valuable insights towards the development of safe, efficient, and sustainable hydrogen technologies.

2.
J Am Chem Soc ; 146(13): 8939-8948, 2024 Apr 03.
Article in English | MEDLINE | ID: mdl-38526452

ABSTRACT

Propane dehydrogenation (PDH) reaction has emerged as one of the most promising propylene production routes due to its high selectivity for propylene and good economic benefits. However, the commercial PDH processes usually rely on expensive platinum-based and poisonous chromium oxide based catalysts. The exploration of cost-effective and ecofriendly PDH catalysts with excellent catalytic activity, propylene selectivity, and stability is of great significance yet remains challenging. Here, we discovered a new active center, i.e., an unsaturated tricoordinated cobalt unit (≡Si-O)CoO(O-Mo) in a molybdenum-doped silicalite-1 zeolite, which afforded an unprecedentedly high propylene formation rate of 22.6 molC3H6 gCo-1 h-1 and apparent rate coefficient of 130 molC3H6 gCo-1 h-1 bar-1 with >99% of propylene selectivity at 550 °C. Such activity is nearly one magnitude higher than that of previously reported Co-based catalysts in which cobalt atoms are commonly tetracoordinated, and even superior to that of most of Pt-based catalysts under similar operating conditions. Density functional theory calculations combined with the state-of-the-art characterizations unravel the role of the unsaturated tricoordinated Co unit in facilitating the C-H bond-breaking of propane and propylene desorption. The present work opens new opportunities for future large-scale industrial PDH production based on inexpensive non-noble metal catalysts.

3.
Opt Lett ; 47(3): 718-721, 2022 Feb 01.
Article in English | MEDLINE | ID: mdl-35103716

ABSTRACT

This paper introduces a fiber-optic microelectromechanical system (MEMS) seismic-grade accelerometer that is fabricated by bulk silicon processing using photoresist/silicon dioxide composite masking technology. The proposed sensor is a silicon flexure accelerometer whose displacement transduction system employs a light intensity detection method based on Fabry-Perot interference (FPI). The FPI cavity is formed between the end surface of the cleaved optical fiber and the gold-surfaced sidewall of the proof mass. The proposed MEMS accelerometer is fabricated by one-step silicon deep reactive ion etching with different depths using the composite mask, among which photoresist is used as the etching-defining mask for patterning the etching area while silicon dioxide is used as the depth-defining mask. Noise evaluation experiment results reveal that the overall noise floor of the fiber-optic MEMS accelerometer is 2.4 ng/H z at 10 Hz with a sensitivity of 3165 V/g, which is lower than that of most reported micromachined optical accelerometers, and the displacement noise floor of the optical displacement transduction system is 208 fm/H z at 10 Hz. Therefore, the proposed MEMS accelerometer is promising for use in high-performance seismic exploration applications.

4.
Sensors (Basel) ; 20(13)2020 Jun 29.
Article in English | MEDLINE | ID: mdl-32610636

ABSTRACT

Temperature sensors are one of the most important types of sensors, and are employed in many applications, including consumer electronics, automobiles and environmental monitoring. Due to the need to simultaneously measure temperature and other physical quantities, it is often desirable to integrate temperature sensors with other physical sensors, including accelerometers. In this study, we introduce an integrated gold-film resistor-type temperature sensor for in situ temperature measurement of a high-precision MEMS accelerometer. Gold was chosen as the material of the temperature sensor, for both its great resistance to oxidation and its better compatibility with our in-house capacitive accelerometer micro-fabrication process. The proposed temperature sensor was first calibrated and then evaluated. Experimental results showed the temperature measurement accuracy to be 0.08 °C; the discrepancies among the sensors were within 0.02 °C; the repeatability within seven days was 0.03 °C; the noise floor was 1 mK/√Hz@0.01 Hz and 100 µK/√Hz@0.5 Hz. The integration test with a MEMS accelerometer showed that by subtracting the temperature effect, the bias stability within 46 h for the accelerometer could be improved from 2.15 µg to 640 ng. This demonstrates the capability of measuring temperature in situ with the potential to eliminate the temperature effects of the MEMS accelerometer through system-level compensation.

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