Highly Advanced Degradation of Thiamethoxam by Synergistic Chemisorption-Catalysis Strategy Using MIL(Fe)/Fe-SPC Composites with Ultrasonic Irradiation

作者：Wei, Yanan; Wang, Bingfeng; Cui, Xinfang; Muhammad, Yaseen; Zhang, Yanjuan; Huang, Zuqiang; Li, Xuesheng; Zhao, Zhenxia; Zhao, Zhongxing

来源：ACS Applied Materials & Interfaces, 2018, 10(41): 35260-35272.

DOI：10.1021/acsami.8b12908

• MIL(Fe)/Fe-SPC catalyst
• efficient charge separation
• thiamethoxam advanced degradation
• DFT simulation
• synergistic chemisorption-catalysis strategy

MIL(Fe)/Fe-doped nanospongy porous biocarbon (Fe-SPC) composite was fabricated from MIL-100(Fe) via in situ growth on a unique Fe-doped nanospongy porous biocarbon (Fe-SPC) and was used as Fenton-like catalyst for advanced degradation of thiamethoxam (THIA). Fe was loaded on silkworm excrement and calcined to Fe-SPC with nanospongy and high sp(2) C structure. The in situ growth strategy embedded the Fe-SPC into MIL-100(Fe) crystals and formed conductive heterojunctions with an intensified interface by Fe-bridging effect, which was confirmed by negative shift of Fe3+ binding energy in X-ray photoelectron spectroscopy. MIL(Fe)/Fe-SPC composites exhibited high degree of crystallinity and surface area (Brunauer-Emmett-Teller: 1730 m(2)/g). Liquid chromatography-mass spectrometry and density functional theory simulations demonstrated that THIA was converted to a relatively stable compound (C4H5N2SCl), which could be captured by MIL-100(Fe) with strong chemical bonding energy (Fe-N, -587 kJ/mol), followed by a significant geometric distortion, resulting in a thorough degradation. Efficient charge separation and synergistic chemisorption-catalysis strategy resulted in the high catalytic activity of MIL(Fe)Fe-SPC. The composite catalyst concurrently exhibited high mineralization ratio with 95.4% total organic carbon removal (at 25 degrees C and 180 min) and good recycling ability under wider neutral/alkaline conditions. Endorsing to these intriguing properties, MIL(Fe)/Fe-SPC can be deemed an efficient contender for removal of hard-degradable pesticides and other environmental pollutants in practical applications.

• 单位
  广西大学; 华南农业大学; 华南热带农业大学