Short‐term effects in a reduced flow stretch: The case of the Antas River in South Brazil

The building of adduction channels (penstocks) that conduct water from reservoirs to turbines, which are located kilometres from the dam, is becoming common, optimizing the electricity generation in small dams. This design creates a river stretch with reduced discharge between the dam and the powerhouse. This study evaluates the short‐term impacts of the below‐dam decrease in river flow on fish assemblages. Samples were collected in the reduced flow stretch of the Castro Alves Hydropower Plant (Antas River, Rio Grande do Sul, Brazil) before the reservoir started operating (January 2008; mean discharge of 103.7 m³/s) and immediately after operation began (March 2008; mean discharge of 12.4 m³/s). Sampling was conducted in distinct habitats of the reduced flow stretch (slow waters—gillnets, sand beaches—seining nets, structured littoral—electrofishing, and fast waters—cast nets) with a strongly standardized effort. The attributes of the fish assemblages were not negatively affected by the flow reduction in any habitat sampled. However, distinct changes in the spatial structure were observed considering the different types of habitat predominantly used by the species, which represents an entire reorganization of the fish assemblages in the short term. It is fundamental that these short‐term aspects be considered in the licensing of hydropower plants in addition to the long‐term changes.     

芽孢杆菌Bacillus sp.dwc-2对模拟地下水中U(Ⅵ)的还原行为研究

在厌氧条件下研究了西南地区一种典型土壤微生物芽孢杆菌Bacillus sp.dwc-2对模拟地下水中U(Ⅵ)的还原行为，重点考察了时间、无机阴离子、腐殖酸（HA）及富里酸（FA）对还原的影响，并利用TEM、EDS、SAED和XPS对还原后的样品进行了表征。结果表明：在pH=7.0、c_NaHCO3=5 mmol/L和T=303 K条件下，Bacillus sp.dwc-2对U(Ⅵ)的还原率随时间的增加而增加，24 h内最大还原率为12.2%，此后则随时间的增加逐渐降低；HA和FA对U(Ⅵ)的微生物还原行为有一定影响，其中HA和FA浓度为25 mg/L时，U(Ⅵ)的还原在24 h最明显，其还原率分别为14.2%和16.2%，但随着HA和FA浓度的继续增加，因在U(Ⅵ)离子与HA、FA形成的配合物表面形成致密的腐殖层，抑制了电子的转移，阻止了U(Ⅵ)的还原。此外，研究表明HCO₃^-也会抑制U(Ⅵ)的还原。TEM-SAED和XPS分析证实了还原过程中U(Ⅳ)的存在。上述结果可为真实环境中微生物还原U(Ⅵ)提供基础数据和参考。     

用于厚屏蔽小探测器的蒙特卡罗模拟减方差方法研究

反应堆屏蔽计算中经常出现厚屏蔽、小探测器问题，常规蒙特卡罗方法难以有效解决。基于自动重要抽样（AIS）方法，本文提出了小探测器自动重要抽样(SDAIS)方法，并针对小探测器问题，优化了AIS方法的虚粒子赌分裂算法。该方法在自主开发的蒙特卡罗屏蔽程序MCShield上进行了实现。使用NUREG/CR-6115 PWR基准题验证该方法的正确性和计算效率。结果表明，SDAIS方法可有效地解决厚屏蔽小探测器问题，相比AIS方法及传统的重要性方法，计算效率提升1~2个量级。     

Crossing the Border: From Keto- to Imine Reduction in Short-Chain Dehydrogenases/Reductases

The family of NAD(P)H-dependent short-chain dehydrogenases/reductases (SDRs) comprises numerous biocatalysts capable of C=O or C=C reduction. The highly homologous noroxomaritidine reductase (NR) from Narcissus sp. aff. pseudonarcissus and Zt_SDR from Zephyranthes treatiae, however, are SDRs with an extended imine substrate scope. Comparison with a similar SDR from Asparagus officinalis (Ao_SDR) exhibiting keto-reducing activity, yet negligible imine-reducing capability, and mining the Short-Chain Dehydrogenase/Reductase Engineering Database indicated that NR and Zt_SDR possess a unique active-site composition among SDRs. Adapting the active site of Ao_SDR accordingly improved its imine-reducing capability. By applying the same strategy, an unrelated SDR from Methylobacterium sp. 77 (M77_SDR) with distinct keto-reducing activity was engineered into a promiscuous enzyme with imine-reducing activity, thereby confirming that the ability to reduce imines can be rationally introduced into members of the “classical” SDR enzyme family. Thus, members of the SDR family could be a promising starting point for protein approaches to generate new imine-reducing enzymes.     

高频氢等离子体增强还原制备超细铜粉

利用高频感应热氢等离子体强化还原制备超细铜粉，考察了加料速率、还原氢气流量、氢气分布位置、反应区空间、冷却温度等因素对铜粉颗粒性能的影响，对制备的铜粉颗粒进行氧含量、XRD晶体结构、松装密度、粒度分布和比表面积的表征。结果表明，优化的工艺条件为反应区内径100 mm，加料速率4 g/min，淬火气氩气气量500 L/h，氢气气量500 L/h并通入少量载气，由氢等离子电离产生的氢自由基可强化反应实现瞬时还原，不仅可控制铜粉形貌，还能有效控制铜粉颗粒大小；利用该方法制备出粒径分布100?200 nm、分散性好的超细球形铜粉颗粒。该方法操作简便、产品纯度高、气氛可控、对环境污染小。     

Oxygen reduction reaction and hydrogen evolution reaction catalyzed by carbon-supported molybdenum-coated palladium nanocubes

Oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) are two important processes for electrochemical energy storage and conversion. Herein, we describe the preparation of carbon-supported Pd nanocubes@Mo core@shell nanostructures as efficient dual catalysts for both ORR and HER. The core@shell structure was manifested by high-resolution transmission electron microscopy measurements, including high angle-angular dark field-scanning transmission electron microscopy and elemental mapping analysis. Further structural insights were obtained in X-ray diffraction and X-ray photoelectron spectroscopy measurements. The nanostructures exhibited apparent electrocatalytic activity toward both ORR and HER, and the performances were markedly higher than those without the deposition of a Mo overlayer. In ORR, the activity was even better than that of commercial Pt/C within the context of onset potential, specific and mass activities; whereas in HER, the performance of Pd nanocubes@Mo core@shell nanostructures remained subpar as compared to that of Pt/C in terms of the overpotential to reach the current density of 10 mA cm^?2, the Tafel slope was comparable and the stability was excellent. The excellent electrocatalytic performance can be attributed to the Pd-Mo synergistic effects imparted from the core-shell structure.     

Role of phosphorus in nitrogen,phosphorus dual-doped ordered mesoporous carbon electrocatalyst for oxygen reduction reaction in alkaline media

In this paper, we have investigated the role of phosphorus (P) in nitrogen (N) and phosphorus dual-doped carbon electrocatalyst for oxygen reduction reaction (ORR) in alkaline media with three samples prepared by varying the doping orders of N and P. Results show that the resultant N-POMC (first doped with P, then N) exhibits an outstanding activity for ORR in alkaline media. The mechanism leading to the improved activity is found to be associated with the orientation effect of the first doped P on the later doped N, by increasing the ratio of graphitic-N significantly. Furthermore, a portion of the first doped P can act as the doping sites and be replaced by the later doped N, called ‘self-sacrifice’ mode, which is confirmed by both experiments and density functional theory (DFT) calculations. However, this orientation effect cannot be observed in the other two dual-doped samples. In addition, experimental and DFT calculation also prove that the amount of graphitic-N is important in improving the activity for ORR. The doping strategy reported in this work is applicable to various co-doping systems in exploring the synergy effect of different dopants and improving activity for ORR.     

Highly Stable COF‐Supported Co/Co(OH)2 Nanoparticles Heterogeneous Catalyst for Reduction of Nitrile/Nitro Compounds under Mild Conditions

Ordered nanoporosity in covalent organic framework (COF) offers excellent opportunity for property development. Loading nanoparticles (nPs) onto them is one approach to introducing tailor‐made properties into a COF. Here, a COF–Co/Co(OH)₂ composite containing about 16 wt% of <6 nm sized Co/Co(OH)₂ nPs is prepared on a N‐rich COF support that catalyzes the release of theoretical equivalence of H₂ from readily available, safe, and cheap NaBH₄. Furthermore, the released H₂ is utilized for the hydrogenation of nitrile and nitro compounds to amines under ambient conditions in a facile one‐pot reaction. The COF “by choice” is built from “methoxy” functionalized dialdehydes which is crucial in enabling the complete retention of the COF structure under the conditions of the catalysis, where the regular Schiff bonds would have hydrolyzed. The N‐rich binding pockets in the COF ensure strong nP–COF interactions, which provides stability and enables catalyst recycling. Modeling studies reveal the crucial role played by the COF in exposing the active facets and thereby in controlling the activation of the reducing agent. Additionally, via density functional theory, we provide a rational explanation for how these COFs can stabilize nanoparticles which grow beyond the limiting pore size of the COF and yet result in a truly stable heterogeneous catalyst – a ubiquitous observation. The study underscores the versatility of COF as a heterogeneous support for developing cheap and highly active nonnoble metal catalysts.