bluuebunny/crossref_metadata_2025_split huggingface dataset:
Simultaneous enhancement of proton conductivity and methanol resistance of sulfonated poly(phthalazinone ether sulfone ketone)/superacid sulfated zirconia composite membranes for direct methanol fuel cells
Authors: Zhen Dongxing , He Gaohong , Xu Xinlong , Yan Xiaoming , Du Naixu , Gong Xue , Li Tiantian , Dai Yan , Wu Xuemei 
Published: August 2018

ABSTRACTSulfonated poly(phthalazinone ether sulfone ketone) (SPPESK) is a kind of novel non‐fluorine polymer, whose high proton conductivity is dependent on high degree of sulfonation, which resulting in loss of dimensional stability. SPPESK/superacid sulfated zirconia (SZrO2) composite proton exchange membranes are fabricated first. The composite membrane shows good dimensional stability, ascribing to the restriction effect of hydrogen bonding force on the mobility and relaxation of polymer chains. Introducing SZrO2simultaneously enhances the conductivity and anti‐methanol permeation, owing to the connected ion domains, enlarged and aggregated ion clusters, excess proton conduction sites, and good blocking effect to methanol of SZrO2. For composite membrane containing 1.5 wt % SZrO2, the highest conductivity of 180 mS cm−1is obtained at 80 °C. Compared with pristine SPPESK and Nafion 115, the methanol permeability is reduced by 54 and 77%, and the maximum power density of direct methanol fuel cell is enhanced by 133 and 25%. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci.2018,135, 46758.
Mechanical properties of poly(3‐hydroxybutyrate‐co‐3‐hydroxyvalerate)/wood flour composites: Effect of interface modifiers
Authors: Chan Clement Matthew , Vandi Luigi‐Jules , Pratt Steven , Halley Peter , Richardson Desmond , Werker Alan , Laycock Bronwyn 
Published: August 2018

ABSTRACTA fully biodegradable and biobased wood plastic composite based on a microbial biopolyester matrix, poly(3‐hydroxybutyrate‐co‐3‐hydroxyvalerate) (PHBV), and a lignocellulosic filler, pine wood flour (WF), was manufactured using extrusion at industry‐standard level of wood content. The effects of three compatibilization techniques on the mechanical properties of the composites were investigated. Techniques include silicone fiber treatment using Sigmacote, maleic anhydride (MA) grafting of PHBV matrix, and the addition of polymethylene diphenyl‐diisocyanate (pMDI). Results showed that Sigmacote treatment resulted in a 20 ± 5% decrease in tensile strength of the composite. The use of MA‐grafted PHBV, independent of content, enhanced slightly the composites tensile strength (5 ± 3%) and impact strength (10 ± 4%). The addition of 2 wt % of pMDI improved the tensile strength of the composite by 25 ± 6%, but the strength level returned to the original state when 4 wt % was added. Processing conditions had a more significant effect on the composite properties giving a 40 ± 5% reduction in tensile strength and 45 ± 6% in impact strength when a higher shear extrusion configuration was used. The modeling of the mechanical data suggested that PHBV/WF composites have achieved better interfacial interactions without compatibilization when compared to other composite systems. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018, 135, 46828.
A sorbitol‐based phase‐selective organogelator for crude oil spills treatment
Authors: Zhuan Cailing , Li Yun , Yuan Xubo , Zhao Jin , Hou Xin 
Published: August 2018

ABSTRACTAn efficient sorbitol‐based phase‐selective organogelator has been synthesized by an one‐step reaction between sorbitol and benzaldehyde with high yields up to 90%. The organogelator could gelate a wide range of oils with minimum gelation concentration ranging from 0.04 to 0.10 g/mL within 17 min. Besides, the self‐assembly mode of the organogelator in the oil phase was presented. The organogelator could self‐assemble in the oil phase through the hydrogen bonding and the π–π stacking interactions to form three‐dimensional networks. The organogelator showed better gelation properties when treated crude oil than other oils. Namely, a lower gelation concentration and a shorter gelling time were observed, while higher thermal stability and mechanical strength of the final crude oil gel were obtained. More importantly, the organogelator could be directly applied in a powder form to selectively gelate crude oil from oil–water mixtures within 10 min at ambient temperature without heating or adding carrier solvents. Inexpensive, simple‐synthesis, high‐yield and relatively simple operation performances of the organogelators indicate their potential and promising applications to remove oil spills in real life, especially for marine crude oil spills. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47052.
Equivalence analyses of dissolution profiles with the Mahalanobis distance
Authors: Hoffelder Thomas 
Published: August 2018

AbstractFor some postapproval changes, the manufacturer has to demonstrate that the dissolution profile of the drug product before the change is statistically equivalent to the dissolution profile after the change. Guidelines suggest the so‐called similarity factor f2 as standard approach for the equivalence analysis. f2 is a statistically questionable transformation of the Euclidean distance between both profile means and does not allow a control of the type I error rate. An alternative multivariate distance measure for quantifying the dissimilarity between both profile groups is the Mahalanobis distance. Current equivalence procedures based on the Mahalanobis distance implicate some practical problems in the dissolution context: either one chooses an exact method but the determination of a product independent equivalence margin will not be practically feasible or one chooses an approximate alternative that suffers from the bias of the Mahalanobis distance point estimate. This paper suggests the T2EQ approach for dissolution profile comparisons. T2EQ is a practically feasible equivalence procedure based on the Mahalanobis distance with an internal equivalence margin for comparing dissolution profiles. The equivalence margin is compliant with current dissolution guidelines. The operating characteristics (size, robustness, and power) are investigated via simulation: T2EQ meets the needs of both authorities and industry: not affected by the bias of the point estimate the type I error rate can be reliably controlled for various distribution assumptions and the power of T2EQ exceeds the power of methods recently discussed in the literature. These results were presented for the first time at CEN‐ISBS 2017.
Aesthetic outcome following breast-conserving surgery assessed by three evaluation modalities in relation to health-related quality of life
Authors: Dahlbäck C , Ringberg A , Manjer J 
Published: August 2018

Abstract

Background
The aim of this study was to compare the agreement between three different methods for evaluation of aesthetic outcome following breast-conserving surgery and adjuvant radiotherapy: a patient questionnaire, panel evaluation of photographs and the software BCCT.core. A further aim was to examine how these modalities predict health-related quality of life as measured by the validated Breast-Q™ questionnaire.

Methods
At 1-year follow-up after breast-conserving surgery, patients completed a study-specific questionnaire. Postoperative photographs were evaluated using the software BCCT.core. A panel of three healthcare professionals assessed preoperative and postoperative photographs. Agreement between methods was assessed using Spearman's correlation coefficients (rs). The Breast-Q™ questionnaire was sent to study participants. The ability of the different evaluation methods to predict Q-scores for the health-related quality-of-life (HRQoL) domains satisfaction with breasts and psychosocial well-being was investigated using receiver operating characteristic (ROC) curves.

Results
A total of 532 patients undergoing breast-conserving surgery were examined before surgery. At 1-year follow-up, 334 patients completed the study-specific questionnaire. Postoperative photographs from 310 patients were evaluated using BCCT.core. The panel of healthcare professionals assessed photographs from 215 patients. Agreement between the different evaluation modalities was poor. The strongest agreement was noted between the panel evaluation for symmetry and BCCT.core results (rs = 0·59, P &lt; 0·001). The Breast-Q™ questionnaire was returned by 348 patients. Patient satisfaction ratings at 1-year follow-up best predicted long-term HRQoL measured using the Breast-Q score, both in terms of satisfaction with breasts (area under the curve (AUC) 0·80, P &lt; 0·001) and psychosocial well-being (AUC 0·73, P &lt; 0·001).

Conclusion
There is currently no ideal method for evaluating aesthetic outcome after breast-conserving surgery and adjuvant radiotherapy. These results emphasize the use of patient-related outcome measures.
The direct and moderating effects of power distance on carbon transparency: An international investigation of cultural value and corporate social responsibility
Authors: Luo Le , Tang Qingliang , Peng Juan 
Published: August 2018

AbstractThere are limited studies on the influence of national culture on corporate social responsibility, and thus, the issue is underexplored. Using an international sample, we show that higher power distance decreases corporate carbon transparency. In addition to this direct effect, we find that power distance also plays a moderating role in the relationship between carbon performance and carbon transparency. We report evidence of a negative association between carbon disclosure and carbon performance in our sample firms, which suggests that disclosure is driven by legitimation purposes. Further findings demonstrate that the tendency toward legitimation is more pronounced in countries with high power distance, which implies that a lower concentration of power promotes corporate social responsibility and reduces carbon opaqueness. Overall, our findings significantly enhance understanding of the role of culture in managerial response to climate change. Such an understanding is extremely important because climate change must be managed by people, and people are influenced by the underlying national cultural preference.
Evidence of Diradicals Involved in the Yeast Transketolase Catalyzed Keto‐Transferring Reactions
Authors: Hsu Ning‐Shian , Wang Yung‐Lin , Lin Kuan‐Hung , Chang Chi‐Fon , Ke Shyue‐Chu , Lyu Syue‐Yi , Hsu Li‐Jen , Li Yi‐Shan , Chen Sheng‐Chia , Wang Kuei‐Chen , Li Tsung‐Lin 
Published: August 2018

AbstractTransketolase (TK) catalyzes a reversible transfer of a two‐carbon (C2) unit between phosphoketose donors and phosphoaldose acceptors, for which the group‐transfer reaction that follows a one‐ or two‐electron mechanism and the force that breaks the C2“−C3” bond of the ketose donors remain unresolved. Herein, we report ultrahigh‐resolution crystal structures of a TK (TKps) from Pichia stipitis in previously undiscovered intermediate states and support a diradical mechanism for a reversible group‐transfer reaction. In conjunction with MS, NMR spectroscopy, EPR and computational analyses, it is concluded that the enzyme‐catalyzed non‐Kekulé diradical cofactor brings about the C2“−C3” bond cleavage/formation for the C2‐unit transfer reaction, for which suppression of activation energy and activation and destabilization of enzymatic intermediates are facilitated.
Role of Organic Components in Electrocatalysis for Renewable Energy Storage
Authors: Liu Gejun , Bai Haipeng , Zhang Bo , Peng Huisheng 
Published: August 2018

AbstractCarbon dioxide electroreduction and water splitting are known as two promising strategies to convert renewable intermittent electrical energy into chemical energy. Thus, the three half‐reactions, namely, CO2 reduction reaction, hydrogen evolution reaction, and the oxygen evolution counter reaction, in these two electrolytic processes have attracted wide research interest. Organic polymer electrocatalysts or electrocatalysts containing organic components play important roles in these catalytic processes. It has been shown that the organic molecules can efficiently catalyze the reactions themselves, and modulate the active sites towards high selectivity and efficiency. The roles of the organic molecules in conducting polymers, the metal complexes, and the framework materials are extracted for the three half‐reactions mentioned above, and this comprehensive review will serve as a guide for future research and aid in the design of electrocatalysts related to organic molecules.
An Omni‐Healable and Highly Sensitive Capacitive Pressure Sensor with Microarray Structure
Authors: Liu Feng , Han Fei , Ling Lei , Li Jinhui , Zhao Songfang , Zhao Tao , Liang Xianwen , Zhu Deliang , Zhang Guoping , Sun Rong , Ho Derek , Wong Ching‐Ping 
Published: August 2018

AbstractCapacitive pressure sensors with high flexibility, sensitivity, and excellent healable properties are desirable for a wide variety of applications, such as e‐skin. However, implementing these characteristics onto a device presently remains a great challenge. In this work, a flexible pressure sensor with high sensitivity and strong healable properties has been developed based on healable polyurethane (HPU), silver nanowires and graphene. The HPU‐based microstructured capacitive pressure sensor exhibited a high sensitivity of 1.9 kPa−1 (<3 kPa), a fast response time (<100 ms), low detection limit (10 Pa), and long‐term durability (1000 cycles). Touch‐finger and vocal‐cord vibration detection have been demonstrated and exhibit a high sensitivity to both static and dynamic pressure. More notably, the entire pressure sensor including the dielectric layer and electrodes is omni‐healable after complete separation. The prototype has experimentally shown tremendous potential for wearable, healable applications, such as healthcare monitoring and human‐machine interfaces.
Sodium‐Doped C3N4/MOF Heterojunction Composites with Tunable Band Structures for Photocatalysis: Interplay between Light Harvesting and Electron Transfer
Authors: Pan Yating , Li Dandan , Jiang Hai‐Long 
Published: August 2018

AbstractThe search for ideal model systems to investigate the role of different parameters in heterojunction composites for enhanced photocatalysis is a high‐priority target. Herein, a series of heterojunction composites, namely Nax‐C3N4/Pt@UiO‐66, being composed of UiO‐66 and Na‐doped g‐C3N4 with adjustable light absorbance and band structures, have been prepared with different Na contents, which exhibit a volcano curve towards photocatalytic H2 production. Benefiting from the interplay of the two critical factors between light harvesting ability and electron transfer efficiency, the optimized Na0.02‐C3N4/Pt@UiO‐66 shows excellent photocatalytic H2 production, far surpassing its corresponding single counterparts.
Spontaneous Substitutions at Phosphorus Trihalides in Imidazolium Halide Ionic Liquids: Grotthuss Diffusion of Anions?
Authors: Hollóczki Oldamur , Wolff Alexander , Pallmann Julia , Whiteside Rachel E. , Hartley Jennifer , Grasser Matthias A. , Nockemann Peter , Brunner Eike , Doert Thomas , Ruck Michael 
Published: August 2018

AbstractPX3 compounds (X=Cl, Br, I) in imidazolium halide ionic liquids combine with the anion Z (Z=Cl, Br, I) of the solvent to form [PX3Z]− complex anions. These anions have a sawhorse shape in which the lone pair of the phosphorus atom fills the third equatorial position of the pseudotrigonal bipyramid. Theoretical results show that this association remains incomplete due to strong hydrogen bonding with the cations of the ionic liquid, which competes with the phosphorus trihalide for interaction with the Z− anion. Temperature‐dependent 31P NMR experiments indicated that the P−Z binding is weaker at higher temperature. Both theory and experiment evidence dynamic exchange of the halide anions at the phosphorus atom, together with continuous switching of the ligands at the phosphorus atom between equatorial and axial positions. Detailed knowledge of the mechanism of the spontaneous exchange of halogen atoms at phosphorus trihalides suggests a way to design novel, highly conducting ionic‐liquid mixtures.
Aggregation of Rare Earth Coordination Complexes in Solution Studied by Paramagnetic and DOSY NMR
Authors: Poh Adeline W. J. , Aguilar Juan A. , Kenwright Alan M. , Mason Kevin , Parker David 
Published: August 2018

AbstractThe degree of aggregation of neutral, 9‐coordinate rare earth coordination complexes has been shown to affect their ligand field, as revealed by diffusion‐ordered NMR spectroscopy (DOSY‐NMR) measurements on Y(III) complexes, paramagnetic NMR analyses of Yb and Tb analogues and emission spectral studies with the EuIII systems. In non‐polar media a lipophilic tris‐isopropyl complex, [Ln.L2] tends to aggregate in chloroform and dichloromethane giving rise to oligomers, whereas in acetic and trifluoroacetic acid the more polar parent complex, [Ln.L1], also aggregates, profoundly affecting the pseudocontact shift and the form of the Eu emission spectrum. Such behaviour has important implications in the design of responsive spectral probes.
Rational Design of a 3D MnII‐Metal–Organic Framework Based on a Nonmetallated Porphyrin Linker for Selective Capture of CO2 and One‐Pot Synthesis of Styrene Carbonates
Authors: Sharma Nayuesh , Dhankhar Sandeep Singh , Kumar Sandeep , Kumar T. J. Dhilip , Nagaraja C. Mallaiah 
Published: August 2018

AbstractA 3D MnII‐porphyrin metal–organic framework (MOF), [{Mn2(TCPP)⋅2H2O}⋅DMF]n (MOF1) (TCPP=5,10,15,20‐tetrakis(4‐benzoate)porphyrin), was constructed; it exhibits an interesting 3D framework structure with two types of 1D channels of dimensions of 3.94×8.37 Å2 and 4.66×4.93 Å2 running along the crystallographic a axis. Owing to the presence of a nonmetallated porphyrin cavity, MOF1 exhibits selective storage of CO2 with an isosteric heat of adsorption value of 32.1 kJ mol−1, which is further supported by theoretical calculations with the calculated binding energy (BE) of 29.78 kJ mol−1. Interestingly, the nonmetallated nature of the porphyrin ligand was exploited for implantation of coordinatively unsaturated FeIII ions to generate a FeIII@MOF1 framework, which acts as an efficient recyclable catalyst for the oxidation of styrenes to the corresponding epoxides in the presence of PhIO as an oxidant at room temperature. Moreover, the one‐pot synthesis of styrene carbonates from styrenes and CO2 was also achieved using FeIII@MOF1 as a catalyst. The rational design of a porous MnII‐porphyrin MOF for the selective capture of CO2 and the one‐pot synthesis of styrene carbonates at mild conditions is reported.
Chemoselective Aerobic Cross‐Dehydrogenative Coupling of Terminal Alkynes with Hydrosilanes by a Nanoporous Gold Catalyst
Authors: Kavthe Rahul D. , Ishikawa Yoshifumi , Kusuma Indra , Asao Naoki 
Published: August 2018

AbstractAerobic cross‐dehydrogenative coupling between terminal alkynes and hydrosilanes occurred in the presence of nanoporous gold catalyst under O2 atmosphere. A variety of alkynylsilanes were synthesized in good‐to‐high yields and the catalyst was easily recovered and reused many times. Furthermore, the chemoselective direct silyl protection of terminal acetylenes of alkynols over the hydroxyl groups was achieved with this catalytic system.
Nitrostyrene‐Modified 2‐(2‐Hydroxyphenyl)benzothiazole: Enol‐Emission Solvatochromism by ESICT‐ESIPT and Aggregation‐Induced Emission Enhancement
Authors: Niu Yahui , Wang Rong , Shao Panlin , Wang Yuxiu , Zhang Yanrong 
Published: August 2018

AbstractExcited‐state intramolecular charge transfer (ESICT) and excited‐state intramolecular proton transfer (ESIPT) are two competitive reactions that occur in the excited states of organic dyes that contain intramolecular hydrogen‐bonds and electron acceptors and donors. Determining the mechanisms of these processes is key to understanding their multiple emission features, as the manner in which these processes interact can be modulated by modifying the dye structure. In addition, donor–π–acceptor (D–π–A) molecules often suffer from aggregation‐induced quenching. Herein, we report the synthesis of three nitrophenyl‐modified 2‐(2‐hydroxyphenyl)benzothiazole (HBT) derivatives, HBT‐s‐NO2, HBT‐d‐NO2, and HBT‐t‐NO2, which have C−C, C=C, and C≡C bonds between their HBT and nitrophenyl moieties, respectively. Compared with the enol emissions from HBT‐s‐NO2 and HBT‐t‐NO2, that from HBT‐d‐NO2 exhibits outstanding solvatochromism owing to consecutive ESICT‐ESIPT. In addition, X‐ray diffraction reveals that despite the highly planar and polar nature of HBT‐d‐NO2, which is strongly H‐aggregated, it exhibits highly efficient fluorescence. Hence, this study provides new insight into the design of ESICT/ESIPT‐coupled systems and for engendering planar dipolar molecules with excellent emission properties in the solid state.
Hybrid Molecular Container Based on Glycoluril and Triptycene: Synthesis, Binding Properties, and Triggered Release
Authors: Liu Wenjin , Lu Xiaoyong , Xue Weijian , Samanta Soumen K. , Zavalij Peter Y. , Meng Zihui , Isaacs Lyle 
Published: August 2018

AbstractInvited for the cover of this issue are the groups of Lyle Isaacs at the University of Maryland and Zihui Meng at the Beijing Institute of Technology. The image depicts the structures of a hybrid water soluble acyclic receptor and bilayer vesicles while CB[6] and PA[5] are fitted in the background to indicate the conceptional relationship between the receptor and CB[n] and PA[n]. Read the full text of the article at 10.1002/chem.201802981.
Exploiting β‐Amino Acid Enolates in Direct Catalytic Diastereo‐ and Enantioselective C−C Bond‐Forming Reactions
Authors: Yu Jin‐Sheng , Noda Hidetoshi , Shibasaki Masakatsu 
Published: August 2018

AbstractIn contrast to the widespread use of α‐amino acid‐equivalent enolates for the preparation of non‐natural amino acids, the utilization of β‐amino‐acid counterparts has been limited. This deficit has resulted in a short supply of β2, 2‐amino acids bearing two substituents at the α‐carbon, especially for peptide synthesis. Herein, racemic 4‐substituted isoxazolidin‐5‐ones were used as precursors of β2‐amino acid enolates in the direct catalytic diastereo‐ and enantioselective C−C bond‐forming reactions, constructing two adjacent stereocenters in a highly stereoselective fashion. The obtained adducts were smoothly coupled with α‐amino acid‐derived α‐ketoacids to afford α/β2, 2‐hybrid dipeptides suitable for 9‐fluorenylmethoxycarbonyl (Fmoc)‐based solid‐phase peptide synthesis. Moreover, the Mannich adducts obtained from isatin‐derived imines were converted to spirocyclic β‐lactams, which have recently received increased attention due to their unique biological activities and conformational preferences.
Organic Salts Suppress Aggregation and Enhance the Hyperpolarizability of a π‐Twisted Chromophore
Authors: Lou Alexander J.‐T. , Righetto Stefania , Cariati Elena , Marks Tobin J. 
Published: August 2018

AbstractTwisted intramolecular charge‐transfer (TICT) chromophores exhibit extraordinary hyperpolarizabilities, β, and are therefore promising for electro‐optic technologies. Nevertheless, centrosymmetric aggregate formation severely diminishes β in concentrated solutions or in polymer matrices. Herein, the remarkable effects of organic salts on the linear and nonlinear optical response of a high β benzimidazolium‐based TICT chromophore, B2TMC‐2, are reported. Addition of Bu4P+Br− to B2TMC‐2 solution in CHCl3 induces a halochromic blueshift, primarily reflecting interactions between Bu4P+Br− and the B2TMC‐2 cationic portion. DC electric‐field induced second‐harmonic generation (EFISH) measurements on B2TMC‐2+Bu4P+Br− solution reveal a large μβ=−22,160×10−48 esu, unprecedented for any chromophore with such a broad optical transparency window. Moreover, Bu4P+Br− is shown to suppress B2TMC‐2 aggregation, thereby preserving high μβ in concentrated solutions. This phenomenon should be applicable to many other NLO chromophores.