作者机构：
[Fengjiao Quan; Pengfei Xu; Xiaolan Chen; Wenjuan Shen; Yun He; Jianfen Li] College of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China;[Falong Jia] College of Chemistry, Central China Normal University, Wuhan 430079, China;[Guangming Zhan] School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
通讯机构：
[Falong Jia] C;College of Chemistry, Central China Normal University, Wuhan 430079, China
摘要：
Nitrate (NO3–) is a widespread pollutant in high-salt wastewater and causes serious harm to human health. Although electrochemical removal of nitrate has been demonstrated to be a promising treatment method, the development of low-cost electro-catalysts is still challenging. In this work, a phosphate modified iron (P-Fe) cathode was prepared for electrochemical removal of nitrate in high-salt wastewater. The phosphate modification greatly improved the activity of iron, and the removal rate of nitrate on P-Fe was three times higher than that on Fe electrode. Further experiments and density functional theory (DFT) calculations demonstrated that the modification of phosphoric acid improved the stability and the activity of the zero-valent iron electrode effectively for NO3– removal. The nitrate was firstly electrochemically reduced to ammonium, and then reacted with the anodic generated hypochlorite to N2. In this study, a strategy was developed to improve the activity and stability of metal electrode for NO3– removal, which opened up a new field for the efficient reduction of NO3– removal by metal electrode materials.
作者机构：
[Zhang, Junjie; Song, Hao; Yang, Haiping; Chen, Hanping; Shao, Jingai; Yu, Jie; Jiang, Hao; Fan, Tingting] Huazhong Univ Sci & Technol, Sch Energy & Power Engn, State Key Lab Coal Combust, Wuhan 430074, Hubei Province, Peoples R China.;[Zhang, Junjie; Chen, Hanping; Shao, Jingai; Jiang, Hao; Fan, Tingting] Huazhong Univ Sci & Technol, Sch Energy & Power Engn, Dept New Energy Sci & Engn, Wuhan 430074, Hubei Province, Peoples R China.;[Li, Jianfen] Wuhan Polytech Univ, Sch Chem & Environm Engn, Wuhan 430023, Hubei, Peoples R China.;[Agblevor, Foster] Utah State Univ, USTAR Bioenergy Ctr, Dept Biol Engn, Logan, UT 84341 USA.;[Zhang, Junjie; Shao, Jingai; Zhang, JJ; Shao, JA] 1037 Luoyu Rd, Wuhan 430074, Hubei, Peoples R China.
通讯机构：
[Zhang, JJ; Shao, JA ] 1;1037 Luoyu Rd, Wuhan 430074, Hubei, Peoples R China.
关键词：
Metal oxide;Molecular dynamics simulation;Monoaromatic hydrocarbons;Volatile desulfurization;Waste tire pyrolysis
摘要：
Pyrolysis can effectively convert waste tires into high-value products. However, the sulfur-containing compounds in pyrolysis oil and gas would significantly reduce the environmental and economic feasibility of this technology. Here, the desulfurization and upgrade of waste tire pyrolysis oil and gas were performed by adding different metal oxides (Fe(2)O(3), CuO, and CaO). Results showed that Fe(2)O(3) exhibited the highest removal efficiency of 87.7% for the sulfur-containing gas at 600°C with an outstanding removal efficiency of 99.5% for H(2)S. CuO and CaO were slightly inferior to Fe(2)O(3), with desulfurization efficiencies of 75.9% and 45.2% in the gas when added at 5%. Fe(2)O(3) also demonstrated a notable efficacy in eliminating benzothiophene, the most abundant sulfur compound in pyrolysis oil, with a removal efficiency of 78.1%. Molecular dynamics simulations and experiments showed that the desulfurization mechanism of Fe(2)O(3) involved the bonding of Fe-S, the breakage of C-S, dehydrogenation and oxygen migration process, which promoted the conversion of Fe(2)O(3) to FeO, FeS and Fe(2)(SO(4))(3). Meanwhile, Fe(2)O(3) enhanced the cyclization and dehydrogenation reaction, facilitating the upgrade of oil and gas (monocyclic aromatics to 57.4% and H(2) to 22.3%). This study may be helpful for the clean and high-value conversion of waste tires.
摘要：
Chemical looping is a promising technology for hydrogen production. Achieving both high purity and yield is an ongoing challenge, due to low fuel conversion and carbon deposition. In this study, a sorption-enhanced chemical looping reforming coupled with water splitting (SE-CLSR-WS) process was proposed to co-produce syngas and H 2 by using waste plastic as the fuel. The Ni-doped Ca 2 Fe 2 O 5 brownmillerites were designed and employed as oxygen carriers (OCs) and CO 2 sorbent. The introduction of Ni leaded to lattice distortion of brownmillerite, thereby enhancing the redox activity of lattice oxygen. In fuel reactor (FR), CaO in-situ captured CO 2 and shifted reaction equilibrium towards PET pyrolysis gas reforming, enhancing both syngas yield and PET conversion rates. Adhere to the surface of OCs, CaO improved cyclic performance by inhibiting agglomeration of active metals. Calcination reactor (CR) was set between FR and steam rector (SR) to in-situ desorb CO 2 and remove carbon deposition, enhancing hydrogen purity in SR. When Ca 2 Ni 0.75 Fe 1.25 O 5 -0.25CaO was applied to SE-CLSR-WS process, it exhibited synergistically strengthened performance in reaction activity, sorption capacity and cyclic stability, with a syngas purity of 82.71 % and H 2 yield of 8.01 mmol/g OC with 93.26 % purity.
摘要：
Ammonia (NH3) can be used as a fertilizer, a chemical or a new generation of fuel and has important agricultural and industrial value. Electrochemical NO3--to-NH3 (NITRR) can realize the conversion of waste into treasure and waste resources, which is a promising method for ammonia synthesis. However, the process of NITRR is very complicated, resulting in product diversification and poor selectivity. In this work, an iron modified cerium oxide in rod form (Fe/CeO2-rod) catalysts was designed and used for the NITRR. The Fe/CeO2-rod catalyst showed excellent activity, and achieves high Faradaic efficiency (FE 95%) and NH3 yield rate (4.04 mg h(-1) cm(-2)) in 0.1 M KOH electrolyte at - 0.52 V versus reversible hydrogen electrode. Furthermore, this catalyst exhibits a negligible activity decay during continuous electrolysis for 25 h. Further experiments provide the important role of Fe, which promote the formation of hydrogen radicals (H*). This study may provide new pathways to improve the activity of inexpensive catalysts for NITRR.
通讯机构：
[Falong Jia; Lizhi Zhang] I;Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, China
关键词：
Ammonia nitrogen removal;Single-atom iron;Non-noble metal catalyst;Aquaculture wastewater
摘要：
Ammonia nitrogen (NH4+-N) is a ubiquitous environmental pollutant, especially in offshore aquaculture systems. Electrochemical oxidation is very promising to remove NH4+-N, but suffers from the use of precious metals anodes. In this work, a robust and cheap electrocatalyst, iron single-atoms distributed in nitrogen-doped carbon (Fe-SAs/N-C), was developed for electrochemical removal of NH4+-N from in wastewater containing chloride. The Fe-SAs/N-C catalyst exhibited superior activity than that of iron nanoparticles loaded carbon (Fe-NPs/N-C), unmodified carbon and conventional Ti/IrO2-TiO2-RuO2 electrodes. And high removal efficiency (> 99%) could be achieved as well as high N-2 selectivity (99.5%) at low current density. Further experiments and density functional theory (DFT) calculations demonstrated the indispensable role of single-atom iron in the promoted generation of chloride derived species for efficient removal of NH4+-N. This study provides promising inexpensive catalysts for NH4+-N removal in aquaculture wastewater. (C) 2022 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.
期刊：
Journal of Soils and Sediments,2023年23(7):2951-2961 ISSN：1439-0108
通讯作者：
Chunlei Song
作者机构：
[Li, Jianfen; He, Yun; Li, Hui; Shen, Wenjuan] Wuhan Polytech Univ, Sch Chem & Environm Engn, Wuhan 430073, Peoples R China.;[Song, Chunlei; Zhou, Yiyong; Cao, Xiuyun] Chinese Acad Sci, Inst Hydrobiol, State Key Lab Freshwater Ecol & Biotechnol, Key Lab Algal Biol, 7 Donghu South Rd, Wuhan 430072, Peoples R China.;[Huang, Daizhong] Ecol & Environm Monitoring Ctr Dongting Lake Hunan, Yueyang 414000, Peoples R China.
通讯机构：
[Chunlei Song] S;State Key Laboratory of Freshwater Ecology and Biotechnology, Key Laboratory of Algal Biology, Institute of Hydrobiology, Chinese Academy of Sciences, Wuhan, People’s Republic of China
摘要：
PurposeSediment internal nutrient loading plays an important role in algal blooms. Thus, understanding the specific characteristics of nutrient (nitrogen (N) and phosphorus (P)) recycling from sediment is important for clarifying the processes and mechanisms of cyanobacterial growth and succession.Materials and methodsSediments and water samples were collected monthly from five sampling sites in Lake Chaohu for 1 year. N and P concentrations in surface and interstitial water were determined, and fractions of sediment organic matter, P, and iron were quantified. P adsorption characteristics were modeled with adsorption isotherms.Results and discussionDolichospermum was the dominant bloom species in the western lake in April, followed by Microcystis from May to September in the whole lake. The impulsive regeneration and release mode from iron-bound P and ammonium (NH4+-N) regeneration from sediment in spring triggered the Dolichospermum bloom. In early summer, continuous P release potential as well as nitrate accumulation and NH4+-N deficiency due to NH4+-N prior assimilation by Dolichospermum jointly drove the transition from Dolichospermum to Microcystis due to the energy saving and competitive advantage of rapid uptake and storage of inorganic P as well as a wide range of N utilization forms for Microcystis. All these facts put the Dolichospermum towards common N and P stress. Furthermore, in summer, NH4+-N rapid regeneration from organic algal detritus remineralization due to the decline of Dolichospermum developed Microcystis blooms.ConclusionsThe specific mode and pathway of N and P recycling from sediment determined the dominant algal species based on the particular N and P utilization strategies of the algae. Pulsed and a vast amount of P release facilitated the Dolichospermum growth, while continuous and a small quantity of P release was in favor of Microcystis growth. Organic N hydrolysis from Dolichospermum detritus further supported the development of a Microcystis bloom.
摘要：
A new benzyls pendant-armed macrobicyclic heterbinuclear Cu(II)-Ni(II) complex has been obtained by template-directed synthesis and characterized by elemental analysis, IR spectra, electrospray mass spectra, and single crystal X-ray diffraction. The complex was bridged by two phenolic oxygens and an acetate radical, with the Cu(II)-Ni(II) distance of 2.9292(8) angstrom. The hydrolytic function, CT-DNA binding and antibacterial properties were also studied. The initial rate values for the hydrolysis of 4-nitophenylphosphate to 4-nitrophenolate by the Cu(II)-Ni(II) complex was 1.33 x 10(-5) s(-1), and 10(4) times faster than that the spontaneous hydrolysis of the phosphate monoester. The complex shows a better binding property to CT-DNA and the intrinsic binding constant is 1.29 x 10(5) M-1. The Stern-Volmer constant is 1.25 x 10(5) M-1. The viscosity increased obviously with the increase of complex concentration, the results showed that the complex bind to DNA through intercalation mode, which was in accordance with the absorption and emission spectral studies. The antibacterial activities against E.coli was also investigated using the Gentamycinas reference system. (C) 2019 Published by Elsevier B.V.
摘要：
A catalyst loaded Ni-Fe using powder active carbon (PAC) and gamma-Al2O3 as the support was prepared for hydrogen-rich syngas production from rape straw pyrolysis in a two-stage fixed reactor. EDX (Energy dispersive X-ray spectroscopy), SEM (Scanning electron microscope) and N-2 isothermal adsorption desorption were used to characterize the catalysts. The results showed that the support of PAC-gamma Al2O3 was uniform with large specific surface area. The metals loaded on the support were well dispersed. The performance of Ni-Fe/PAC-gamma Al2O3 catalysts compared with single support catalyst NiO-Fe2O3/gamma Al2O3 (NFA) and NiO-Fe2O3/PAC (NFP) was studied. The results showed that the Ni-Fe/PAC-gamma Al2O3 catalysts showed a good catalytic activity which obviously enhanced the H-2 gas yield to 54.23 g/kg Rape straw and reduced the tar yield to 4.06 g/kg. Meanwhile, Ni-Fe/PAC-gamma Al2O3 catalysts had a stronger ability to prevent the deactivation to keep a longtime stability than the single carrier catalyst. (C) 2019 Elsevier Ltd. All rights reserved.
摘要：
A new macrocyclic heterobinuclear Cu(II)-Zn(II) complex was synthesized and characterized by elemental analysis, FT-IR, ES-MS, and single-crystal X-ray diffraction. Five-coordinate geometry for the new complex is proposed. The copper horizontal ellipsis zinc distance bridged by two phenolic oxygens and a acetate ligand is 2.9508 angstrom. The phosphate ester hydrolysis activity and the DNA binding ability of the complex were studied. The results showed that the present complex has an efficient catalytic activity of phosphoester bond cleavage. The catalytic rate constant k(cat) for the hydrolysis of 4-nitrophenyl phosphate disodium salt hexahydrate (pNPP) by the synthesized complex is 2.69 x 10(-4) s(-1) and 10(5) times faster than the spontaneous hydrolysis of the phosphate monoester. The complex shows a good binding ability to calf thymus (CT-DNA) and the corresponding binding constant is 1.9 x 10(5) M-1. The linear Stern-Volmer quenching constant obtained by the fluorescent spectroscopic is 6.3 x 10(4) M-1. [GRAPHICS] .
