石英ESR法在河流沉积物源示踪中的探讨及应用

使用石英ESR法示踪河流沉积物源是一种新方法和新理论的探索。本文从拟解决的科学问题出发,在着重分析石英ESR信号强度和CI值物源示踪理论基础之上,讨论了该方法在亚洲现代沙尘沉降物源示踪和地质历史时期风尘堆积物源示踪研究中的有效性,结合ESR测年可覆盖整个第四纪时期的特性,认为石英ESR法不仅可以为物源示踪提供良好的年代框架约束,而且还可以较好的反映地质历史时期沉积物质来源在不同时空尺度上的变化特征。随后,通过对指导思想、研究思路以及长江流域不同河段和主要支流的地质地貌背景、岩石类型分布、水系组合特征以及"源-汇"系统之间物质剥蚀-堆积过程的可通达性等方面的综合论述与分析,讨论了石英ESR法在河流沉积物源示踪上的有效性及其在研究长江流域水系发育历史和沉积演化过程中的可行性。     

A simple method to harness DC (direct current) electrical energy generated by bacterial activity

We developed a new system for collecting electrons generated by bacterial activity to supply DC (direct current) electrical energy. This system used eight titanium sub-electrodes (surface area of each sub-electrode: 189 cm²) connected to one central main titanium electrode (surface area of electrode: 1571 cm²). The distance between each sub-electrode and the main electrode was 30 cm. In an initial experiment, we collected electrons during composting cattle excreta, which was mixed with a commercially available microbial compost activator/starter. We analysed the relationships between the composting temperature and electrical current and voltage. Electrons were effectively collected and used successfully to obtain DC electrical energy. Generation of a stable voltage of approximately 0.5 V was clearly observed. This voltage was not related to compost temperature; however, the generated electrical current increased and decreased with compost temperature. The method was then used in a second experiment to collect electrons generated by bacterial activity in an agricultural field (area: 48 m²). Electrons in the field were effectively collected, and we measured a stable voltage of approximately 1.1 V and a stable current of approximately 0.7 mA. The system has the advantages of being simple, easily maintained, inexpensive, and applicable to large-scale agricultural fields.     

Size fractionation and characterization of nanocolloidal particles in soils

A protocol was developed to fractionate soil particles down to the nanocolloid scale by combining sieving, sedimentation, centrifugation, and cross-flow filtration (CFF). The validity of the method and the performance of the CFF system were tested by characterizing fractions using laser granulometry, electron microscopy, and chemical analysis. The 0.1-μm-pore-size membrane CFF system effectively retained nanocolloids (<0.1 μm) as shown by laser granulometry and observed directly by transmission electron microscopy. However, environmental scanning electron microscopy images of freeze-dried colloids were very different from their TEM counterparts, suggesting that sample preparation influenced microscopy imaging. Chemical analysis of Cu, Cd, and organic carbon in each fraction showed that the concentrations of these components increased as particle size decreased, indicating colloids and nanocolloids play an important role in retaining trace metals. Particle-size fractionation combined with chemical analysis and electron microscopy can provide insight into the nature and properties of nanocolloids in soil.     

Enhanced catalytic oxidation of 2,4-dichlorophenol via singlet oxygen dominated peroxymonosulfate activation on CoOOH@Bi2O3 composite

• Bi₂O₃ cannot directly activate PMS. • Bi₂O₃ loading increased the specific surface area and conductivity of CoOOH. • Larger specific surface area provided more active sites for PMS activation. • Faster electron transfer rate promoted the generation of reactive oxygen species. • ¹O₂ was identified as dominant ROS in the CoOOH@Bi₂O₃/PMS system. Cobalt oxyhydroxide (CoOOH) has been turned out to be a high-efficiency catalyst for peroxymonosulfate (PMS) activation. In this study, CoOOH was loaded on bismuth oxide (Bi₂O₃) using a facile chemical precipitation process to improve its catalytic activity and stability. The result showed that the catalytic performance on the 2,4-dichlorophenol (2,4-DCP) degradation was significantly enhanced with only 11 wt% Bi₂O₃ loading. The degradation rate in the CoOOH@Bi₂O₃/PMS system (0.2011 min⁻¹) was nearly 6.0 times higher than that in the CoOOH/PMS system (0.0337 min⁻¹). Furthermore, CoOOH@Bi₂O₃ displayed better stability with less Co ions leaching (16.4% lower than CoOOH) in the PMS system. These phenomena were attributed to the Bi₂O₃ loading which significantly increased the conductivity and specific surface area of the CoOOH@Bi₂O₃ composite. Faster electron transfer facilitated the redox reaction of Co (III) / Co (II) and thus was more favorable for reactive oxygen species (ROS) generation. Meanwhile, larger specific surface area furnished more active sites for PMS activation. More importantly, there were both non-radical (¹O₂) and radicals (SO₄⁻•, O₂⁻•, and OH•) in the CoOOH@Bi₂O₃/PMS system and ¹O₂ was the dominant one. In general, this study provided a simple and practical strategy to enhance the catalytic activity and stability of cobalt oxyhydroxide in the PMS system.     

Isolation,identification, and the degradation characteristics of a BDE-47 degrading strain北大核心CSCD

In an effort to remove BDE-47 residues from the environment, a bacterial strain that is capable of utilizing BDE-47 as the sole carbon source was isolated and screened from soil collected from an e-waste recycling area in Tianjin to analyze the degradation properties. The strain was preliminarily identified as Enterobacter sp. according to a 16S rDNA gene sequence analysis. The strain degraded 35.8% of 525 μg/L of BDE-47 in 35 d when the initial concentration of bacteria was 7.1 × 105 cells/ mL. The product of the biodegradation of BDE-47 was BDE-28. The biodegradation of BDE-47 fit well with first-order kinetics, and its degradation kinetics was ln Ct = - 0.104t + 6.22. With the addition of an electron acceptor, such as Fe3+, SO4 2- and NO3 -, the BDE-47 degradation rate was significantly increased to 49.8%, 59.1%, and 67.3%, respectively. The above results revealed that the strain could degrade BDE-47, which is of importance in the application of environmental bioremediation of BDE-47. © 2018 Science Press. All rights reserved.     

Enhancement of extracellular Cr(VI) reduction for anammox recovery using hydrazine: performance,pathways, and mechanism

● N₂H₄ addition enhanced and recovered anammox performance under Cr(VI) stress. ● N₂H₄ accelerated electron transfer of Cr(VI) reduction for detoxification. ● N₂H₄ enhanced anammox metabolism for activity recovery from Cr(VI) inhibition. ● Extracellular Cr(VI) reduction to less toxic Cr(III) was the dominant mechanism. The hexavalent chromium (Cr(VI)) would frequently impose inhibition to anaerobic ammonium oxidation (anammox) process, hindering the efficiency of nitrogen removal in wastewater treatment. Hydrazine (N₂H₄), which is an intermediate product of anammox, participates in intracellular metabolism and extracellular Cr(VI) reduction. However, the roles of N₂H₄-induced intracellular metabolism and extracellular reduction in nitrogen removal under Cr(VI) stress remain unclear. The addition of 3.67 mg/L of N₂H₄ increased the anammox activity by 17%. As an intermediate, N₂H₄ enhanced anammox metabolism by increasing the heme c content and electron transfer system activity. As a reductant, N₂H₄ accelerated the reduction of c-Cyts-mediated extracellular Cr(VI) to the less toxic Cr(III). Extracellular Cr(III) accounts for 74% of the total Cr in a Cr(VI)-stressed anammox consortia. These findings highlight that N₂H₄-induced extracellular Cr(VI) reduction is the dominant mechanism for the survival of anammox consortia. We also found that N₂H₄ increased the production of extracellular polymeric substances to sequester excessive Cr(VI) and produced Cr(III). Taken together, the study findings suggest a potential strategy for enhancing nitrogen removal from ammonium-rich wastewater contaminated with Cr(VI).     

Utilizing transparent and conductive SnO2 as electron mediator to enhance the photocatalytic performance of Z-scheme Si-SnO2-TiOx

• A novel Z-scheme Si-SnO₂-TiO_x with SnO₂ as electron mediator is first constructed. • Transparent and conductive SnO₂ can pass light through and promote charge transport. • V_O from SnO₂ and TiO_x improve photoelectrochemical performances. • Efficient photocatalytic degradations originate from the Z scheme construction. Z-scheme photocatalysts, with strong redox ability, have a great potential for pollutants degradation. However, it is challenging to construct efficient Z-scheme photocatalysts because of their poor interfacial charge separation. Herein, by employing transparent and conductive SnO₂ as electron mediator to pass light through and promote interfacial charge transportation, a novel Z-scheme photocatalyst Si-SnO₂-TiO_{x (1<x<2)} was constructed. The Z-scheme photocatalyst displayed an order of magnitude higher photocurrent density and a 4-fold increase in open-circuit potential compared to those of Si. Moreover, the onset potential shifted negatively for approximately 2.2 V. Benefiting from these advantages, this Z-scheme Si-SnO₂-TiO_x exhibited efficient photocatalytic performance toward phenol degradation and mineralization. 75% of the phenol was degraded without bias potential and 70% of the TOC was removed during phenol degradation. Other typical pollutants such as bisphenol A and atrazine could also be degraded without bias potential. Introducing a transparent and conductive electron mediator to construct Z-scheme photocatalyst gives a new sight to the improvement of photocatalytic performance in Z scheme.     

Dual-reaction-center catalytic process continues Fenton’s story

• Dual-reaction-center (DRC) system breaks through bottleneck of Fenton reaction. • Utilization of intrinsic electrons of pollutants is realized in DRC system. • DRC catalytic process well continues Fenton’s story. Triggered by global water quality safety issues, the research on wastewater treatment and water purification technology has been greatly developed in recent years. The Fenton technology is particularly powerful due to the rapid attack on pollutants by the generated hydroxyl radicals (•OH). However, both heterogeneous and homogeneous Fenton/Fenton-like technologies follow the classical reaction mechanism, which depends on the oxidation and reduction of the transition metal ions at single sites. So even after a century of development, this reaction still suffers from its inherent bottlenecks in practical application. In recent years, our group has been focusing on studying a novel heterogeneous Fenton catalytic process, and we developed the dual-reaction-center (DRC) system for the first time. In the DRC system, H₂O₂ and O₂ can be efficiently reduced to reactive oxygen species (ROS) in electron-rich centers, while pollutants are captured and oxidized by the electron-deficient centers. The obtained electrons from pollutants are diverted to the electron-rich centers through bonding bridges. This process breaks through the classic Fenton mechanism, and improves the performance and efficiency of pollutant removal in a wide pH range. Here, we provide a brief overview of Fenton’s story and focus on combing the discovery and development of the DRC technology and mechanism in recent years. The construction of the DRC and its performance in the pollutant degradation and interfacial reaction process are described in detail. We look forward to bringing a new perspective to continue Fenton’s story through research and development of DRC technology.     

Elevated CO2 response of photosynthesis depends on ozone concentration in aspen

The effect of elevated CO₂ and O₃ on apparent quantum yield (?), maximum photosynthesis (P_max), carboxylation efficiency (V_cmax) and electron transport capacity (J_max) at different canopy locations was studied in two aspen (Populus tremuloides) clones of contrasting O₃ tolerance. Local light climate at every leaf was characterized as fraction of above-canopy photosynthetic photon flux density (%PPFD). Elevated CO₂ alone did not affect ? or P_max, and increased J_max in the O₃-sensitive, but not in the O₃-tolerant clone. Elevated O₃ decreased leaf chlorophyll content and all photosynthetic parameters, particularly in the lower canopy, and the negative impact of O₃ increased through time. Significant interaction effect, whereby the negative impact of elevated O₃ was exaggerated by elevated CO₂ was seen in Chl, N and J_max, and occurred in both O₃-tolerant and O₃-sensitive clones. The clonal differences in the level of CO₂ × O₃ interaction suggest a relationship between photosynthetic acclimation and background O₃ concentration.     

One-electron standard reduction potentials of nitroaromatic and cyclic nitramine explosives

Extensive studies have been conducted in the past decades to predict the environmental abiotic and biotic redox fate of nitroaromatic and nitramine explosives. However, surprisingly little information is available on one-electron standard reduction potentials (E^o(R-NO₂/R-NO₂⁻)). The E^o(R-NO₂/R-NO₂⁻) is an essential thermodynamic parameter for predicting the rate and extent of reductive transformation for energetic residues. In this study, experimental (linear free energy relationships) and theoretical (ab initio calculation) approaches were employed to determine E^o(R-NO₂/R-NO₂⁻) for nitroaromatic, (caged) cyclic nitramine, and nitroimino explosives that are found in military installations or are emerging contaminants. The results indicate a close agreement between experimental and theoretical E^o(R-NO₂/R-NO₂⁻) and suggest a key trend: E^o(R-NO₂/R-NO₂⁻) value decreases from di- and tri-nitroaromatic (e.g., 2,4-dinitroanisole) to nitramine (e.g., RDX) to nitroimino compound (e.g., nitroguanidine). The observed trend in E^o(R-NO₂/R-NO₂⁻) agrees with reported rate trends for reductive degradation, suggesting a thermodynamic control on the reduction rate under anoxic/suboxic conditions.