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JOURNAL OF MEMBRANE SCIENCE · 2022 · IF 10.53

Hydrophobically modified Pd membrane for the efficient purification of hydrogen in light alcohols steam reforming process

Chenyang Zhao,Yujia Liu,Hongwei Zhu,Junjie Feng,Huiyun Jiang,Fei An,Yan Jin,Wei Xu,Zhe Yang,Bing Sun

The ability to selectively remove H 2 from the product has made palladium (Pd) membrane reactor a good choice for steam reforming reaction. However, carbonaceous deposited on the surface of Pd membrane during reaction hindered its industrial application. In order to protect Pd membrane from being poisoned by water and light alcohols, a TS-1/Pd composite membrane was prepared by a facile one-step hydrothermal method combined with silane coupling treatment. The zeolite layer acted as a protective armor by keeping poisonous species away from the Pd bulk, and the silanization process increased the hydrophobicity by reducing the hydroxyl density on the surface of TS-1/Pd composite membrane. After 100 h’s exposure in the steam reforming condition, the percentage of carbon content was only 0.95% for the TS-1/Pd membrane, compared with 13.20% for the pure Pd membrane. The H 2 permeability and H 2 /N 2 selectivity of the TS-1/Pd remained constant, while that for pure Pd membrane fell by 50% and 80%, respectively. The significantly improved resistance to carbon deposition provides possibility for the large-scale application of Pd membrane reactor in hydrogen production via steam reforming.

研究领域: 化学工程 · 材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2023 · IF 7.2

Efficient processing of tritiated water by using a two-stage Pd membrane reactor with Pt/TiO2 catalyst

Lei Yue,Linjie Zhao,Jingwei Hou,Junyan Wang,Jiamao Li,Chengjian Xiao

Large amounts of tritiated water (HTO) will be produced during the operation of nuclear power plants and fusion devices, which is harmful to the environment and human due to its radioactivity and toxicity. So, the tritium concentration of tritiated water must be reduced to a very low value before discharge. Hydrogen-water isotope exchange reaction (H 2  + HTO→H 2 O + HT) based on palladium membrane reactor has been proposed to process tritiated water. However, a comprehensive study about the influence of operation parameters on the membrane reactor performance is insufficient, which is not conducive to the design of reactor in practical application. Moreover, the commonly used Pt/Al 2 O 3 or Ni/SiO 2 catalysts are not active for tritiated water dissociation, so the catalytic activity of these catalysts is not high. In order to process tritiated water more effectively, a two-stage membrane reactor has been designed and established in this work, and Pt/TiO 2 catalyst with rich oxygen vacancies is used to catalyze the hydrogen-water isotope exchange reaction for the first time. The membrane reactor performance shows an approximate linear relationship with a new combined parameter S 0.5 P 1.5 R / F 2 ( S is membrane area , F is water flow rate , P is vapor partial pressure, R is swamping ratio), which can be used predict the membrane performance . The isotope exchange reaction activity of Pt/TiO 2 is better than that of Pt/Al 2 O 3 due to its good ability for water dissociation and the hydrogen spillover effect. At last, a tritiated water processing experiment by using two-stage membrane reactor with Pt/TiO 2 catalyst with rich oxygen vacancies has been carried out. The tritium decontamination factor reaches 40588, which is the highest experimental value so far. The results indicate that the two-stage Pd membrane reactor based on hydrogen-water isotope exchange reaction is an efficient technology for tritiated water processing.

CAS / MDL: 13463-67-7 16941-12-1
研究领域: 环境科学 · 核能工程 · 催化化学
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-10 · IF 16.6

Electrochemistry-assisted selective butadiene hydrogenation with water

Yan Yong-Qing,Chen Ya,Wang Zhao,Chen Li-Hua,Tang Hao-Lin,Su Bao-Lian

Alkene feedstocks are used to produce polymers with a market expected to reach 128.4 million metric tons by 2027. Butadiene is one of the impurities poisoning alkene polymerization catalysts and is usually removed by thermocatalytic selective hydrogenation. Excessive use of H 2 , poor alkene selectivity and high operating temperature (e.g. up to 350 °C) remain the most significant drawbacks of the thermocatalytic process, calling for innovative alternatives. Here we report a room-temperature (25~30 °C) electrochemistry-assisted selective hydrogenation process in a gas-fed fixed bed reactor, using water as the hydrogen source. Using a palladium membrane as the catalyst, this process offers a robust catalytic performance for selective butadiene hydrogenation, with alkene selectivity staying around 92% at a butadiene conversion above 97% for over 360 h of time on stream. The overall energy consumption of this process is 0.003 Wh/mL butadiene , which is thousands of times lower than that of the thermocatalytic route. This study proposes an alternative electrochemical technology for industrial hydrogenation without the need for elevated temperature and hydrogen gas.

CAS / MDL: 7697-37-2 1310-58-3
研究领域: 化学工程 · 电化学 · 催化 · 材料科学
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Nature Water · 2023 ·Vol. 1 ·期 1 ·95-103 · IF 0

Electrochemical hydrogenation of oxidized contaminants for water purification without supporting electrolyte

Xu Yinghua,Mao Zhechuan,Qu Ruifeng,Wang Jisheng,Yu Jianming,Luo Xingyu,Shi Meiqin,Mao Xinbiao,Ding Jie,Liu Bin

Electrocatalytic hydrogenation enables the efficient treatment of oxidized contaminants in water under mild conditions, but its application has been greatly hindered by the need for a supporting electrolyte and the large amounts of unsafe intermediate products. Here we report the development of a rhodium nanoparticle-modified palladium membrane electrochemical reactor (Rh NPs-PdMER) for the hydrogenation of oxidized contaminants in drinking water and industrial effluents. The Rh NPs-PdMER not only enabled the hydrogenation of 12 different oxidized contaminants to safe products with ≥99% conversion and ≥95% yield in water without a supporting electrolyte, but also required a very low operating voltage of only 1.4 V. The performance of the Rh NPs-PdMER can be attributed to the specific reactor configuration and the unique adsorbability of the hydrogenated intermediates of the oxidized contaminants to the Rh nanoparticles.

研究领域: 环境科学 · 水处理技术 · 电化学 · 纳米材料
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Interstitial boron-doped nanoporous palladium film for electro-reduction of nitrogen to ammonia

Ziqiang Wang,Min Li,Peng Wang,Kai Deng,Hongjie Yu,Xin Wang,You Xu,Hongjing Wang,Liang Wang

Electrocatalytic nitrogen reduction to ammonia has attracted abundant research interest due to its mild operation condition and sustainable feedstock. The identification of efficient catalysts with high selectivity of nitrogen reduction is the key for the electro-synthesis of ammonia. Herein, interstitial boron-doped nanoporous palladium film is directly formed on Ni foam (nPdB/NF) via micelle-assisted reduction method using borane dimethylamine complex as reducing agents and boron dopant. The binder-free nanoporous structure provides abundant active sites and facilitated mass/charge transfer. Moreover, the introduction of interstitial boron atoms can modify the electronic structure of Pd, which can both improve the nitrogen adsorption and inhibit hydrogen evolution on nPdB/NF. As such, nPdB/NF exhibits high NH 3 yield of 29.0 μg h −1 mg −1 cat. and Faraday efficiency of 17.9% in 0.1 M Na 2 SO 4 , superior to that of nPd/NF (19.7 μg h −1 mg −1 cat and 14.7%). This work offers an attractive method for the introduction of interstitial boron into Pd-based catalysts to improve NRR performance.

研究领域: 电化学 · 催化 · 材料科学 · 可持续化学
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