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| 1 | Atmospheric heterogeneous reaction of chlorobenzene on mineralα-Fe_(2)O_(3)particulates:a chamber experiment study显示文摘Despite the large emission of chlorinated volatile organic compounds(CVOCs)into the atmosphere,the ultimate fate of these compounds remains largely unknown.Herein,we explore the photochemical conversion of an important class of CVOCs,namely chlorobenzene(CB),on mineralα-Fe_(2)O_(3)particulates under atmospheric relevant conditions.A series of chamber reactions composed of the CB with/without SO_(2)or NO_(2)are performed,followed by in situ diffuse reflectance infrared Fourier transform spectroscopy measurements and density functional theory calculations.We show that CB can be considerably degraded byα-Fe_(2)O_(3)under light irradiation,whereas the reaction is markedly suppressed by adding SO_(2)or NO_(2)owing to their competitive adsorption and surface acidification.In particular,we discover that CB can be ultimately converted into polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)under dark state or light irradiation,suggesting a possible origin of atmospheric PCDD/Fs from this overlooked photochemical source. | Meiling Chen Mengjie Yin Yuetan Su Ruizhe Li Kezhou Liu Zhongbiao Wu Xiaole Weng | 2023 | Frontiers of Environmental Science & Engineering2023，17，11： | 0 |
| 2 | Catalytic destruction of chlorobenzene over K-OMS-2: Inhibition of high toxic byproducts via phosphate modification显示文摘In the process of catalytic destruction of chlorinated volatile organic compounds(CVOCs),the catalyst is prone to chlorine poisoning and produce polychlorinated byproducts with high toxicity and persistence,bringing great risk to atmospheric environment and human health.To solve these problems,this work applied phosphate to modify K-OMS-2 catalysts.The physicochemical properties of catalysts were determined by using X-ray powder diffraction(XRD),scanning electron microscope(SEM),X-ray photoelectron spectroscopy(XPS),hydrogen temperature programmed reduction(H_(2)-TPR),pyridine adsorption Fouriertransform infrared(Py-IR)and water temperature programmed desorption(H_(2)O-TPD),and chlorobenzene was selected as a model pollutant to explore the catalytic performance and byproduct inhibition function of phosphating.Experimental results revealed that 1 wt.%phosphate modification yielded the best catalytic activity for chlorobenzene destruction,with the 90%conversion(T90)at approximately 247℃.The phosphating significantly decreased the types and yields of polychlorinated byproducts in effluent.After phosphating,we observed significant hydroxyl groups on catalyst surface,and the active centerwas transformed into Mn(IV)-O…H,which promoted the formation of HCl,and enhanced the dechlorination process.Furthermore,the enriched Lewis acid sites by phosphating profoundly enhanced the deep oxidation ability of the catalyst,which promoted a rapid oxidation of reaction intermediates,so as to reduce byproducts generation.This study provided an effective strategy for inhibiting the toxic byproducts for the catalytic destruction of chlorinated organics. | Yunpeng Long Jiajia Liu Meiling Chen Renna Li Xiaole Weng Zhongbiao Wu | 2023 | Journal of Environmental Sciences2023，，5： | 0 |
| 3 | A simple hydroxypyridine ionic liquids for conversion of CO_(2)into quinazoline-2,4(1H,3H)-diones under atmospheric conditions显示文摘The transformation of CO_(2)into high value-added product is a promising pathway for utilizing CO_(2).However,the process tends to require harsh reaction conditions owing to CO_(2)chemical inertness.Designing a high efficiency catalytic system with environmentally benign characteristic are important determinants.In this work,protic ionic liquids[TMG][2-OPy]were prepared via one-step neutralization between 1,1,3,3-tetramethylguanidine and 2-hydroxypyridine,applying to the domain of synthesizing quinzoline-2,4(1 H,3H)-diones from CO_(2)and 2-aminobenzontiles without any solvent or metal,achieving the yield of 97%at 90℃for 8 h under atmospheric.A series of substrates with good to acceptable yield were detected,revealing the generality and universality of the catalyst.Furthermore,the system could be facilely reused for at least six runs,retaining the yield of 94%.A preliminary kinetic equation is calculated with the activation energy of 68 kJ·mol^(-1),and a plausible reaction mechanism was put forward.This study highlights that the[TMG][2-OPy]enables to activate CO_(2)carboxylation efficiently. | Bowen Jiang Meiling Weng Jigang An Yuewei Fan Jia Liu Ying Liu Ting Yu Leizhi zheng Guoqiang Yang Zhibing Zhang | 2023 | Chinese Journal of Chemical Engineering2023，62，10： | 0 |
| 4 | Distinct but correct:generating diversified and entity-revised medical response显示文摘Medical dialogue generation(MDG)is applied for building medical dialogue systems for intelligent consultation.Such systems can communicate with patients in real time,thereby improving the efficiency of clinical diagnosis.However,predicting correct entities and correctly generating distinct responses remain a great challenge.Inspired by actual doctors'responses to patients,we consider MDG a two-stage task:entity prediction and dialogue generation.For entity prediction,we design an ent-mac post pre-training strategy by leveraging external medical entity knowledge to enhance the pre-trained model.For dialogue generation,we propose an entity-aware fusion MDG method in which predicted entities are integrated into the dialogue generation model through different encoding fusion mechanisms,using information from different sources.Because the diverse beam search algorithm can produce responses with entities that deviate from the predicted entities,an entity-revised diverse beam search is proposed to correct the entities entailed in the generated responses and make the generated responses more distinct.The experimental results on the China Conference on Knowledge Graph and Semantic Computing 2021(A/B tests)and the International Conference on Learning Representations 2021(online test)datasets show that the proposed method outperforms several state-of-the-art methods,which demonstrates its practicability and effectiveness. | Bin LI Bin SUN Shutao LI Encheng CHEN Hongru LIU Yixuan WENG Yongping BAI Meiling HU | 2024 | Science China(Information Sciences)2024，67，3： | 0 |
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