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MXene/MnO_(2)对有机微污染物的类芬顿氧化降解效能与机理
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作者 文涛 郭思胜 +6 位作者 赵恒新 郑宇琦 张馨月 顾鹏程 张塞 艾玥洁 王祥科 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第6期215-225,共11页
芬顿高级氧化技术是降解有机微污染物的有效手段.过一硫酸盐(PMS)类芬顿技术因具有高效的氧化剂利用率和较宽的pH操作范围,已成为目前工业中过氧化氢芬顿技术的一种有前途的替代品.非均相催化剂能够有效活化PMS,产生多种活性自由基,从... 芬顿高级氧化技术是降解有机微污染物的有效手段.过一硫酸盐(PMS)类芬顿技术因具有高效的氧化剂利用率和较宽的pH操作范围,已成为目前工业中过氧化氢芬顿技术的一种有前途的替代品.非均相催化剂能够有效活化PMS,产生多种活性自由基,从而氧化降解有机微污染物.二维过渡金属碳化物/氮化物(MXene)具有较好的电子传输效率和可调的表面官能团,是一种良好的非均相催化材料.然而,MXene的不稳定性、反应体系的自聚集作用和不明确的活性氧(ROS)生成机制极大地限制了它们在实际环境中的广泛应用.鉴于剥离的MXene中钛的高反应活性缺陷可以原位锚定过渡金属材料,本文通过氧化还原策略,将MnO_(2)纳米颗粒原位沉积在MXene纳米片上制备了MXene/MnO_(2)复合材料.X射线衍射图中(002)峰的偏移、透射电镜和电子衍射环图中交错的晶格条纹等表征结果表明,MnO_(2)纳米颗粒均匀地负载在剥离的MXene纳米片上.X射线光电子能谱证实了MXene表面钛缺陷与MnO_(2)纳米颗粒通过氧化还原作用相连接.同时,通过调整反应时间确定了18 h原位沉积制备的MXene/MnO_(2)具有最佳的产率和双酚A降解速率.此时的复合材料能够在4 min内活化PMS去除95.9%的BPA(50 mg/L),矿化效率达到了51.2%,表现出较好的催化性能.电子顺磁共振和淬灭实验结果表明,MXene/MnO_(2)活化PMS降解BPA为非自由基途径.实验观察结合密度泛函理论计算表明,大量暴露的锰位点有效吸附并活化PMS,从而促进了单线态氧的产生.通过高价Mn-oxo相直接生成1O_(2)的普遍途径具有较高的能垒(3.34 eV).相比之下,•OOH作为中间体产生1O_(2)的途径(1.84 eV)在能量上更可行.得益于MXene的快速电荷转移能力和MnO_(2)强PMS活化能力的双重优势,工程化的MXene/MnO_(2)/PVDF催化膜对京密引水渠河水中的有机微污染物表现出高效的活性和出色的长期稳定性.综上,本文通过氧化还原原位生长策略制得了MXene/MnO_(2)催化剂,并深入研究了其在类芬顿反应中催化降解有机微污染物的性能.通过实验表征和理论计算相结合的方法,揭示了该催化剂对有机微污染物的降解机理.本研究不仅为MXene基催化剂的设计和合成提供了新的思路,也为开发可广泛应用于实际水体中处理有机微污染物的催化剂提供了参考. 展开更多
关键词 MXene 二氧化锰 过一硫酸盐 单线态氧 类芬顿反应
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Novel Radiation-Adjustable Heating Terminal Based on Flat Heat Pipe Combined with Air Source Heat Pump
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作者 Yifan Wu Hongli Sun +3 位作者 Mengfan Duan Borong Lin hengxin zhao Chaohung Liu 《Engineering》 SCIE EI CAS CSCD 2023年第1期192-207,共16页
The electrification of building heating is an effective way to meet the global carbon target. As a clean and sustainable electrified heating technology, air-source heat pumps (ASHPs) are widely used in areas lacking c... The electrification of building heating is an effective way to meet the global carbon target. As a clean and sustainable electrified heating technology, air-source heat pumps (ASHPs) are widely used in areas lacking central heating. However, as a major component of space heating, heating terminals might not fit well with ASHP in order to achieve both intermittency and comfort. Therefore, this study proposes a novel radiation-adjustable heating terminal combined with an ASHP to achieve electrification, intermittency, and better thermal comfort. Radiant terminals currently suffer from three major problems: limited maximum heating capacity, inability to freely adapt, and difficulty with combining them with ASHPs. These problems were solved by improving the structural design of the novel terminal (Improvement A–E). Results showed that the maximum heating capacity increased by 23.6% and radiation heat transfer ratio from 10.1% to 30.9% was provided for users with the novel terminal. Further, new flat heat pipe (FHP) design improved stability (compressor oil return), intermittency (refrigerant thermal inertia), and safety (refrigerant leakage risk) by reducing the length of exposed refrigerant pipes. Furthermore, a new phased operation strategy was proposed for the novel terminal, and the adjustability of the terminal was improved. The results can be used as reference information for decarbonizing buildings by electrifying heating terminals. 展开更多
关键词 Novel heating terminal Air-source heat pump Structural impr ovement design Maximum heating capacity Rapid adjustability Room temperature distribution
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