Directed Evolution of a Cp*RhIII-Linked Biohybrid Catalyst Based on a Screening Platform with Affinity Purification

Directed evolution of Cp*Rh^III-linked nitrobindin (NB), a biohybrid catalyst, was performed based on an in vitro screening approach. A key aspect of this effort was the establishment of a high-throughput screening (HTS) platform that involves an affinity purification step employing a starch-agarose resin for a maltose binding protein (MBP) tag. The HTS platform enables efficient preparation of the purified MBP-tagged biohybrid catalysts in a 96-well format and eliminates background influence of the host E. coli cells. Three rounds of directed evolution and screening of more than 4000 clones yielded a Cp*Rh^III-linked NB(T98H/L100K/K127E) variant with a 4.9-fold enhanced activity for the cycloaddition of acetophenone oximes with alkynes. It is confirmed that this HTS platform for directed evolution provides an efficient strategy for generating highly active biohybrid catalysts incorporating a synthetic metal cofactor.     

One‐shot radical polymerization of vinyl monomers with different reactivity accompanying spontaneous delay of polymerization for the synthesis of double‐network hydrogels

Double‐network hydrogels were conveniently synthesized by the one‐shot radical polymerization of an ionic monomer for the first network and a non‐ionic monomer for the second network in the presence of crosslinkers by simultaneous addition of the monomers, that is, one‐shot and spontaneous two‐step polymerization accompanying the delay of polymerization of a second network monomer. We analyzed the polymerization process based on the conversion of each monomer during the reaction in the absence of crosslinkers. Then we fabricated the double‐network hydrogels using several polymerization systems consisting of a conjugated monomer and a non‐conjugated monomer in the presence of the dual crosslinkers. We analyzed the swelling, mechanical and viscoelastic properties of hydrogels synthesized by one‐shot radical polymerization to confirm the production mechanism and the network structure of the hydrogels. © 2020 Society of Chemical Industry     

Effects of Using Alternative Extreme Pressure (EP) and Anti-Wear (AW) Additives with Oxy-Nitrided Samples

Oxy-nitriding is a widely used industrial process aiming to improve the tribological properties and performance of components. Previous studies have shown the effectiveness of the treatment with friction and wear performance, but very few have focussed on optimising this behaviour. The lubrication properties of several EP and AW additives were examined to investigate their effectiveness in improving the tribological properties of the layers formed after treatment. Previous studies showed the presence of an oxide layer on the sample could improve the effectiveness of the sulphurised olefin (SO) and tricresyl phosphate (TCP) additives. The friction and wear behaviour of oxy-nitrided samples were analysed using a tribometer and surface profiler. Scanning electron microscope, energy-dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy were employed to identify the morphologies and chemical compositions of the treated surface before and after testing. No real effect on friction was observed when using the SO or TCP additives, mostly due to lack of interaction with the less reactive iron nitride layer and their roles as anti-wear additives. However, when the zinc dialkyldithiophosphate-containing lubricant was used, a higher friction coefficient was observed. Greater improvements in anti-wear properties with the presence of additives in comparison with only using base oil were reported, with the TCP additive producing the lowest wear rates. The study effectively demonstrated that the additive package type used could impact the tribological and tribochemical properties of oxy-nitrided surfaces.     

Site‐Selective Iron(III) Chloride‐Catalyzed Arylation of 4‐Aryl‐4‐methoxy‐2,5‐cyclohexadienones for the Synthesis of Polyarylated Phenols

The iron(III) chloride‐catalyzed Friedel–Crafts arylation of 4‐aryl‐4‐methoxy‐2,5‐cyclohexadienones, which were easily prepared by the phenyliodine(III) diacetate (PIDA)‐mediated oxidation of 4‐arylphenols in methanol, proceeded site‐selectively to form meta‐terphenyl (2,4‐diarylphenol) derivatives in good yields. The subsequent PIDA‐mediated oxidation and iron(III) chloride‐catalyzed Friedel–Crafts arylation of the resulting products gave the corresponding 2,4,6‐triarylphenol derivatives. The present method provides useful highly substituted polyarylated compounds.

     

Flexible manipulator inspired by octopus: development of soft arms using sponge and experiment for grasping various objects

In this study, we focus on the intelligent behavior of an octopus and describe the development of a flexible manipulator. To realize the intelligent behavior, we employ sponges, rubbers and wires instead of electrical computers. The manipulator is controlled by the dynamics of the body such as the flexibility of the sponges, resilience of the rubbers and constraint by the wires. To demonstrate the effectiveness of the proposed manipulator, we conducted experiment for grasping various objects. We confirmed that grasping behaviors similar to those of an octopus can be realized by the dynamics of the body without electrical computers.     

A Two‐Stage Stochastic Mixed‐Integer Programming Approach to the Smart House Scheduling Problem

A “smart house” is a highly energy‐optimized house equipped with photovoltaic (PV) systems, electric battery systems, fuel cell (FC) cogeneration systems, electric vehicles (EVs), and so on. Smart houses are attracting much attention recently because of their enhanced ability to save energy by making full use of renewable energy and by achieving power grid stability despite an increased power draw for installed PV systems. Yet running a smart house's power system, with its multiple power sources and power storages, is no simple task. In this paper, we consider the problem of power scheduling for a smart house with a PV system, an FC cogeneration system, and an EV. We formulate the problem as a mixed‐integer programming problem, and then extend it to a stochastic programming problem involving recourse costs to cope with uncertain electricity demand, heat demand, and PV power generation. Using our method, we seek to achieve the optimal power schedule running at the minimum expected operation cost. We present some results of numerical experiments with data on real‐life demands and PV power generation to show the effectiveness of our method. © 2013 Wiley Periodicals, Inc. Electr Eng Jpn, 186(4): 48–58, 2014; Published online in Wiley Online Library ( wileyonlinelibrary.com ). DOI 10.1002/eej.22336     

Can land use regulations and taxes help mitigate vehicular CO2 emissions? An empirical study of Japanese cities

This study advocates a multi-dimensional urban planning strategy to help combat climate change under local—and not national—policies. However, the literature does not provide adequate guidance to local governments seeking to enhance urbanization and in turn reduce vehicular carbon dioxide (CO₂) emissions. Therefore, this study sheds light on the effects of the following four urban planning instruments on vehicular CO₂ emissions: urbanization promoting areas, urbanization control areas, urban planning taxes and property taxes. Using Japanese city-level data from 1990 to 2010, we find that the two urbanization area planning instruments and the urban planning taxes help lower emissions by increasing population density in low-density cities and that property taxes help reduce emissions in high-density cities. However, the increased population density associated with these instruments can lead to other negative outcomes, including increased traffic accidents, increased crime and a decrease in the facility condition index. City governments should consider complementary policies to mitigate such negative outcomes when employing planning instruments aiming to increase population density.