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Water · 2017 ·Vol. 9 ·期 8 ·563 · IF 1.832

Study on Effects of Electron Donors on Phosphine Production from Anaerobic Activated Sludge

Jianping Cao,Chaosheng Zhang,Hongwei Rong,Meihua Zhao,Wei Wei,Limin Zhao

The effects of different types and concentrations of electron donors (glucose, starch, methanol and sodium acetate) on the formation of phosphine from anaerobic activated sludge that has been domesticated for a prolonged period were studied in small batch experiments. The results show that types and concentrations of electron donor have significant effects on the production of phosphine from anaerobic activated sludge. Among them, glucose was the most favourable electron donor, whereas sodium acetate was the least favourable electron donor for the removal of phosphorus and the production of phosphine. Higher concentrations of electron donors were more favourable for the reduction of phosphate into phosphine, and supplying more than nine times the amount of electron donor as theoretically required for the reduction of phosphate into phosphine was favourable for the production of phosphine.Keywords:anaerobic activated sludge;electron donor;phosphine;matrix-bound phosphine (MBP)

研究领域: 环境生物学 · 废水处理
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WATER AIR AND SOIL POLLUTION · 2025 ·Vol. 236 ·期 10 ·1-13 · IF 3

Facile Synthesis of Support-Free Copper-Based Catalyst for PH3 Catalytic Oxidation in Micro-Oxygen

Li Yuan,Fan Jun,Huang Bingyao,Li Hongyan,Zhao Jie,Li Kai,Wang Fei

Removal of PH 3 from industrial gases have attracted extensive attention due to its high toxicity and catalyst poisoning characteristics. In this study, a series of copper-based support-free catalysts were synthesized by a facile method using different nitrogen and carbon sources. The 100% removal of PH 3 could reach 540 min in micro-oxygen environment by using the obtained catalyst. The X-ray diffractometer (XRD) and X-ray photoelectron spectroscopy (XPS) results exhibited that the formation of Cu 3 P was contributed to the deactivation of the catalysts, which was considered as active component for the decomposition of PH 3 . The PH 3 decomposition performance could achieve 99% under 450 ℃ with 90% yield of H 2 using the exhausted catalysts. This strategy is beneficial for the development of dephosphorization catalyst and provides a new route for the secondary use of exhausted catalysts. Graphical A facile strategy was employed for synthesize support-free catalysts for PH3 oxidation by using Cu(NO3)2 and different nitrogen resources or carbon resource. The performance were thoroughly compared. The exhausted catalyst was conducted in the PH3 catalytic dissociation reaction, where the conversion rate of PH3 could reach 99% with 90% hydrogen production under 450 ℃.

研究领域: 环境催化 · 材料科学 · 工业气体净化 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Synergistic role of Co and CoP on highly dispersed cobalt nanoparticles embeded in porous carbon for efficient PH3 decomposition

Bingyao Huang,Fei Wang,Hongyan Li,Yuan Li,Kai Li

Efficient resourceful treatment of phosphine tail gas is a huge challenge. In this study, a series of cobalt nanoparticles embeded in porous carbon (Co@C) catalysts were obtained via pyrolysis of Co-based MOF as precursor for catalytic decomposition of phosphine (PH 3 ) by regulating the ratio of reactants of MOFs. The composition, morphology and structure of the catalysts were characterized by inductively coupled plasma, X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy and BET measurement. The effect of Co@C catalysts with different reactant ratio on the catalytic decomposition of PH 3 was tested, and the catalysts before and after the reaction were compared. It was found that the catalyst with MOF as the precursor after pyrolysis can still retain the porosity and large specific surface area of MOF. The metal cobalt nanoparticles and its oxides can be uniformly distributed in time under high loading, which is conducive to the reaction with phosphine to form metal phosphide (CoP), and the rapid and efficient decomposition of PH 3 was completed under the synergistic effect of the two kinds of active sites of Co and CoP. The best catalytic decomposition efficiency is Co@C-5 catalyst, which can achieve 100 % decomposition efficiency at 350 °C and has good stability.

CAS / MDL: 10026-22-9 67-56-1
研究领域: 催化材料 · 环境科学 · 化学工程
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CHEMISTRY OF MATERIALS · 2024 · IF 7.2

Pressure-Induced Multistep Dehydrogenated Polymerization and Metallization of H2S–PH3–H2 Compound: Properties Measurement up to Megabar Pressures

Xiangdong Li,Kangchi Zhang,Wentao Liang,Cheng Zhong,Di Mai,Azizur Rahman,Xiaoyu Sun,Rucheng Dai,Zhongping Wang,Qiang Wu,Zengming Zhang

Recently, hydrogen sulfide (H2S) and phosphine (PH3) have attracted great attention since the observation of superconducting transitions with high crucial temperatures under high pressure, which inspired subsequent investigations of the superconductivity of nonmetallic hydrides. Here, we report the successful photochemical and thermal syntheses of a series of novel H2S–PH3–H2 ternary hydrides with varying H2S and PH3 molar ratios. Raman, infrared, UV–visible absorption spectra, and electrical transport measurements are employed to investigate the chemical reaction and electronic structure transformation under high pressure. The pressure-induced polymerization of PH3 can be confirmed in H2S–PH3–H2 by Raman and infrared spectra, and the polymerization product, P4H6, can be recovered to ambient pressure; additionally, the polymerization pressure of PH3 is evidently hampered with increasing H2S concentration. Furthermore, it has been found that low temperatures can significantly inhibit the pressure-induced polymerization of PH3. The formation of Hittorf’s phosphorus is experimentally confirmed upon unloading pressure from 100 GPa to ambient pressure, which strongly implies the decomposition of P4H6 under high pressure. The H2S–PH3–H2 molecule gradually turns red and is eventually opaque following compression, which is consistent with the red shift of the UV–visible absorption spectra. Furthermore, synchrotron infrared absorption spectra and electrical transport examined above 65 GPa indicate the insulator-to-metal transition of H2S–PH3–H2 caused by dehydrogenated polymerization of P4H6 to Hittorf’s phosphorus.

CAS / MDL: 7704-34-9
研究领域: 材料科学 · 凝聚态物理 · 超导研究
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Ce-doping CuO/HZSM-5 as a regenerable sorbent for Adsorption–Oxidation removal of PH3 at low temperature

Jiayu Feng,Fei Wang,Chi Wang,Kai Li,Ping Ning,Xin Sun,Lijuan Jia

A series Ce m Cu n O x /HZSM-5 sorbents were introduced to remove PH 3 in low-temperature and low-oxygen environments. The effects of copper loading and cerium doping on the adsorption–oxidation performance of the sorbents were investigated. Experimental results showed that doping with 1 wt% of cerium (Ce 1 Cu 30 O X /HZSM-5) could significantly improve the performance of the sorbent. The PH 3 breakthrough capacity was identified as 114.36 mg(PH 3 )•g sorbent -1 . In addition, after three thermal regeneration cycles, the sorbent still has ideal performance. X-ray diffractometer (XRD) and X-ray photoelectron spectroscopy (XPS) analyses exhibited that CuO was the main active species, and Ce-doping can increase the chemisorption oxygen on the surface of the sorbent. BET results demonstrated that the introduction of cerium could improve the specific surface area and pore volume of sorbent. Hydrogen temperature-programmed reduction (H 2 -TPR) and scanning electron microscope (SEM-EDS) indicated that cerium species played an important role in uniformly dispersing copper species on the HZSM-5 surface and improving the oxidation performance of sorbent. Moreover, the reaction products and mechanisms were also investigated by XRD, XPS, and in-situ FTIR spectra. The results indicated that the consumption of CuO and the accumulation of phosphorus species (e.g., P, P 2 O 5 , and Cu 3 P) on the surface and inner pores of the sorbent were the primary reasons for the deactivation of the sorbent.

研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2017 · IF 3.359

Mechanism of PH3 absorption by Cu+-ILs/H2O two-liquid phase system

Guangfei Qu,Qian Zhao,Ronglong Jian,Junya Wang,Dianxin Liu,Ping Ning

Beginning with the formation of the ionic liquid/water two-liquid phase catalytic system for absorption of PH 3 , we designed and synthesized Cu + -[Bmim]PF 6 , which has a hydrophobic property, and later formed a two-liquid phase system with Cu + -[Bmim]PF 6 and water, which has high PH 3 absorption efficiency, and an effective separation of the product and the catalyst was achieved. The effects of temperature and O 2 concentration on phosphine absorption, and the distribution of catalytic components and products in the ionic liquid/aqueous two-phase system were studied. Moreover, the mechanism of Cu + -ILs/water two-liquid phase catalytic oxidation of phosphine was discussed based on results from the analysis of FT-IR and ion chromatography . The results demonstrated that the optimum oxygen content in the reaction was 3%, and the optimum reaction temperature was 45   °C. Cu + -ILs/water two-liquid phase system has a high absorption efficiency for PH 3 , the absorption process is liquid phase catalytic oxidation and the product is H 3 PO 4 . The two-liquid phase system is semi-intelligent. The system can achieve high performance liquid phase catalytic oxidation of PH 3 , as well as automatic separation of H 3 PO 4 .

CAS / MDL: 109-69-3 616-47-7
研究领域: 化学工程 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

Properties of AC and 13X zeolite modified with CuCl2 and Cu(NO3)2 in phosphine removal and the adsorptive mechanisms

Xuanwen Xu,Guoqiang Huang,Shuai Qi

Adsorbents including CuCl 2 -AC, CuCl 2 -13X, Cu(NO 3 ) 2 -AC and Cu(NO 3 ) 2 -13X were prepared to remove trace phosphine from recycled hydrogen in the Siemens process of producing polysilicon , and adsorptive mechanisms were determined by X-ray diffraction and intermittent breakthrough experiments. CuCl 2 could disperse better on supporters than Cu(NO 3 ) 2 , and it existed in its original form. However, Cu(NO 3 ) 2 decomposed into copper oxide or basic cupric nitrate, and showed conspicuous thermal aggregation effect after calcination . Interactive effects between cupric components and supporters varied form species to species and deactivated the reactivity of CuCl 2 and Cu(NO 3 ) 2 in different degree, which resulted in disparities of adsorbents’ performances. CuCl 2 -AC and Cu(NO 3 ) 2 -AC had better performances than CuCl 2 -13X and Cu(NO 3 ) 2 -13X because cupric components were deactivated more when loaded on 13X zeolite. Chemical transformation of phosphine made adsorbents’ surface renewable, and the renewed rate depended on the reactivity of cupric components. All of adsorbents showed significant recoveries of efficiencies in intermittent experiments.

CAS / MDL: 10125-13-0 10031-43-3
研究领域: 材料科学 · 环境工程
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JOURNAL OF HAZARDOUS MATERIALS · 2020 · IF 9.038

Mitigation the release of toxic PH3 and the fire hazard of PA6/AHP composite by MOFs

Yuyang Li,Xiangmei Li,Ye-Tang Pan,Xingyan Xu,Yunze Song,Rongjie Yang

Aluminum hypophosphite (AHP) is a high-efficiency phosphorus-based flame retardant with high P content, which is widely used in Polyamide 6 (PA6). However, AHP releases phosphine gas (PH 3 ) at high temperatures, which is highly toxic to human’s health and environment. Metal-organic frameworks (MOFs) have porous structure exhibiting high performance in gas adsorption. Therefore, mesoporous iron (III) carboxylate [MIL-100 (Fe)] was synthesized in this work and employed to study the adsorption capacity of toxic PH 3 in PA6/AHP composite during processing. AHP was combined with melamine cyanurate (MCA) and MIL-100 (Fe) followed by blending with PA6 to prepare PA6 composites (PA6/MA and PA6/MAF). PA6/MAF with the weight ratio of 5:5 performed well in inhibiting the release of PH 3 during the processing of composite as well as the accelerated thermal experiment devised by our group. Besides, PA6/MAF (5:5) showed relatively low fire hazard reflected by the reduction of the peak of heat release rate of PA6 composite from 962 to 260 kW/m 2 compared with that of pure PA6 in the cone calorimeter test, and MIL-100 (Fe) along with MCA also presented synergistic effect in suppressing the emission of carbon monoxide. The subtle selection of MOFs herein has the potential to be used as a promising synergist for hazardous gases released from polymer composites to improve the occupational and fire safety in the society.

CAS / MDL: 108-78-1 554-95-0
研究领域: 材料科学 · 环境科学 · 化学工程
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SENSORS AND ACTUATORS B-CHEMICAL · 2022 · IF 9.221

A fluorescent detection pen for sensitive, specific, and real-time detection of phosgene based on a novel rhodamine probe

Yingying Li,Jie Zhang,Zengqiang Liang,Ran Yang,Lingbo Qu,Zhaohui Li,Yuanqiang Sun

It is of great significance for real-time monitoring of phosgene to protect public safety. In this paper, a new rhodamine derivate with highly rapid, special and sensitive response towards phosgene was synthesized and used as a phosgene probe based on its spirolactam ring-opening property and nucleophilic reaction with phosgene. To realize in situ visualization of phosgene, a fluorescent detection pen with gas-liquid reaction model was proposed for the first time using the mixture of the probe and polystyrene as ink. The detection film could be formed in situ by simply writing on desired surface and respond toward phosgene gas within 30 s with an ultra-low detection limit (2 ppm) with the naked eye. Such a fluorescence pen detection mode supplied a new strategy for the fabrication of an excellent platform for real-time detection of phosgene and other gas analytes.

研究领域: 化学 · 环境科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Highly stable phosphine modified VOx/Al2O3 catalyst in propane dehydrogenation

Yu Gu,Haijun Liu,Miaomiao Yang,Zhipeng Ma,Lianming Zhao,Wei Xing,Pingping Wu,Xinmei Liu,Svetlana Mintova,Peng Bai,Zifeng Yan

The relatively low cost and mild toxicity of vanadium makes it an alternative to commercially applied Pt and Cr based catalysts in propane dehydrogenation (PDH). Conventional VO x /Al 2 O 3 catalyst shows high initial activity, but deactivates fast due to severe coke formation, which requires frequent regeneration by coke combustion and causes massive CO 2 emissions. In this context, we report on the phosphine (PH 3 ) surface modification of VO x /Al 2 O 3 catalyst leading to substantial improvement of its stability. The phosphorus considerably modifies the properties of the VO x /Al 2 O 3 catalyst: (i) tunes surface acidity, (ii) separates polymerized vanadium oxide species and (iii) weakens interaction between vanadium species with alumina support. Synergy among all these factors facilitates desorption of produced propylene and inhibit the oligomerization of coke precursors, which contributed to the enhancement of the catalyst stability during propane dehydrogenation.

研究领域: 化学工程 · 催化材料科学
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Polymers · 2024 ·Vol. 16 ·期 20 ·2946 · IF 4.7

Preparation of Montmorillonite–Melamine Cyanurate and Inhibition of the Emission of Phosphine from PA6/Aluminum Hypophosphate

Lin Wang,Yuyang Li,Chenyang Yan,Xiangmei Li,Jiyu He,Rongjie Yang

In order to mitigate the release of toxic phosphine from aluminum hypophosphite in twin-screw processing, montmorillonite–melamine cyanurate was prepared by three methods: (1) mechanical intercalation, (2) water intercalation and (3) in situ intercalation. The sheet spacing of montmorillonite was increased from 1.140 nm to 1.141 nm, 1.208 nm and 1.217 nm for these three methods, respectively, and scanning electron microscope (SEM) and transmission electron microscopy (TEM) proved that melamine cyanurate was successfully inserted into the montmorillonite sheets. The montmorillonite–melamine cyanurate from in situ intercalation can best inhibit the release of PH3from aluminum hypophosphite, and the peaks of phosphine, mean values of phosphine and integral of phosphine were reduced by 81.9%, 72.1% and 72.2%, respectively. The mode of action of montmorillonite–melamine cyanuric inhibition of the emission of phosphine from aluminum hypophosphite can be attributed to the physical absorption of montmorillonite and the chemical bonding of melamine cyanurate. In addition, in situ intercalation can slightly improve flame retardancy, attributed to incomplete exfoliation of montmorillonite sheets.

研究领域: 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

The Cu/TiO2 adsorbent modified by Ce-doping removes trace phosphorus impurities from circular hydrogen of a polysilicon chemical vapor deposition furnace

Ze Luo,Qingxin Liang,Yuanshuai Qi,Guoqiang Huang

There is an urgent need for efficient and cost-effective adsorbents for the removal of trace hydrogen phosphide (PH 3 ) from the circular hydrogen systems in the polysilicon chemical vapor deposition furnaces. In this study, a straightforward and cost-effective method was used to synthesize a highly efficient adsorbent (Ce x -Cu y /TiO 2 ) for PH 3 removal using TiO 2 as the carrier and CuO as the active substance. Experimental findings demonstrated that optimal Ce doping amounts (n Cu :n Ce  = 20:1) markedly enhanced the adsorbent's performance, with an adsorption capacity reaching as high as 149.14 mg g −1 . Material characterization results indicated that Ce positively influenced the uniform dispersion of Cu on the TiO 2 surface, and Ce doping increased the adsorbed oxygen content of the adsorbent, consequently enhancing its oxidation performance. The investigation of the reaction mechanism and causes of adsorbent deactivation revealed that the depletion of active substances (CuO) in the adsorbent and the accumulation of products such as Cu 3 P and phosphates are the primary factors contributing to its deactivation. Furthermore, high-temperature calcination could restore the activity of the adsorbent, indicating its great potential for engineering applications.

CAS / MDL: 13463-67-7
研究领域: 化学工程 · 材料科学 · 环境科学
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