Increased Energy Efficiency Using Pulse-potential Electrochemical Advanced Oxidation Processes.

The research investigated the pulse potential effect on Electrochemical Advanced Oxidation Processes (EAOPs) for benzoic acid oxidation. The current efficiency of the electrooxidation is enhanced by changing the pulse frequency and potential on electrodes. The experiments showed that there are opposing phenomena affecting energy efficiency. On the one hand, pulse potential accelerates the mass transfer of benzoic acid in an electric field. On the other hand, pulse potential increases the non-faradic current that uses energy without causing oxidation. Using the Sand equation and the electric double-layer theory, we optimized the pulse frequency and voltage amplitude to achieve the highest energy efficiency for the pulse potential EAOPs. Compared with DC (Direct current) EAOPs, the pulse potential EAOPs save 50% EE/O and have a 41 % CE for the 4_2 V cycle at 50 Hz. Therefore, pulse potential EAOPs can achieve both high pollutant degradation efficiency and low energy consumption at the same time.

Repeatedly Programmable Liquid Crystal Dielectric Elastomer with Multimodal Actuation.

Dielectric elastomers (DEs) are actuatable under an electric field, whose large strain and fast response speed compare favorably with natural muscles. However, the actuation of DE-based devices is generally limited to a single mode and cannot be reconfigured after fabrication, which pales in comparison to biological counterparts given the ability to alter actuation modes according to external conditions. To address this, liquid crystal dielectric elastomers (LC-DEs) that can alter the dielectric actuation modes based on the thermally triggered shape-changing are prepared. Specifically, the two shapes through the LC phase transition possess different bending stiffness, which leads to distinct actuation modes after an electric field is applied. Moreover, the two shapes can be individually programmed/reprogrammed, that is, the one before the transition is regulated through force-directed solvent evaporation and the one after the transition is via bond exchange-enabled stress relaxation. As such, the multimodal dielectric actuation behaviors upon temperature change can be readily diversified. Meanwhile, the space charge mechanism endows LC-DEs with the significantly reduced driving e-field (8 V µm-1) and bidirectional actuation manners. It is believed this unique adaptivity in the actuation modes under a low electric field shall offer versatile designs for practical soft robots.

Hydrogel Rivet with Unidirectional Shape Morphing for Flexible Mechanical Assembly.

Integrating diverse materials and functions into highly additive produce has piqued global interest due to the increasing demands of intelligent soft robotics. Nevertheless, existing assembly techniques, especially supramolecular assembly which heavily rely on precise chemical design and specific recognition, may prove inadequate when confronted with diverse external demands. Inspired by the traditional mechanical assembly, rivet connection, herein, a thermo-responsive hydrogel with unidirectional shape-morphing is fabricated and a stable mechanical assembly is constructed by emulating the rivet connection mechanism. This system employed poly(acrylamide-co-acrylic acid) [P(AAm-co-AAc)] to induce continuous swelling and hexylamine-modified polyvinyl alcohol (PVA-C6) as a molecular switch to control the swelling process. The hydrogel rivet, initially threaded through pre-fabricated hollows in two components. Subsequently, upon the disassociation of alkane chains the molecular switch would activate, inducing swelling and stable mechanical assembly via anchor structures. Moreover, to enhance the assembly strength, knots are introduced to enhance assembly strength, guiding localized stress release for programmed deformations. Additionally, the system can be remotely controlled using near-infrared light (NIR) by incorporating photo-thermal nanoparticles. This work presents a universal and efficient strategy for constructing stable mechanical assemblies without compromising overall softness, offering significant potential for the fabrication of integrated soft robots.

Microstructured Gel Polymer Electrolyte and an Interdigital Electrode-Based Iontronic Barometric Pressure Sensor with High Resolution over a Broad Range.

We present a novel iontronic barometric pressure sensor based on a gel polymer electrolyte and interdigital electrodes with a much simpler structure than that of existing devices. By introducing high-density microstructures on the gel polymer electrolyte and one side electrode arrangement configuration, the developed sensor offers high performances with an ultrahigh resolution of 10 Pa, an ultrawide barometric pressure-response range from -92 to 7 kPa, a fast response time of ∼15 ms, and excellent long-term stability. The single pressure sensor is able to detect positive and negative barometric pressures without needing any additional means and can operate as a barometric altimeter with a resolution of about one-floor height. The performances of the sensors significantly surpass those of existing barometric pressure sensors. This work provides a new strategy for making high-performance barometric pressure sensors that are highly sought for commercial applications such as altitude detection, negative pressure ambulance, and consumer electronics.

Tunable Folding Assembly Strategy for Soft Pneumatic Actuators.

With intrinsic compliance, soft pneumatic actuators are widely utilized in delicate tasks. However, complex fabrication approaches and limited tunability are still problems. Here, we propose a tunable folding assembly strategy to design and fabricate soft pneumatic actuators called FASPAs (folding assembly soft pneumatic actuators). A FASPA consists only of a folded silicone tube constrained by rubber bands. By designing local stiffness and folding manner, the FASPA can be designed to achieve four configurations, pure bending, discontinuous-curvature bending, helix, and discontinuous-curvature helix. Analytical models are developed to predict the deformation and the tip trajectory of different configurations. Meanwhile, experiments are performed to verify the models. The stiffness, load capacity, output force, and step response are measured, and fatigue tests are performed. Further, grippers with single, double, and triple fingers are assembled by utilizing different types of FASPAs. As such, objects with different shapes, sizes, and weights can be easily grasped. The folding assembly strategy is a promising method to design and fabricate soft robots with complex configurations to complete tough tasks in harsh environments.

What is the role of interface in the catalytic elimination of multi-carbon air pollutants?

Multi-carbon air pollutants pose serious hazards to the environment and health, especially soot and volatile organic compounds (VOCs). Catalytic oxidation is one of the most effective technologies for eliminating them. The oxidation of soot and most hydrocarbon VOCs begins with C-H (or edge-CH) activation, so this commonality can be targeted to design active sites. Rationally designed interface nanostructures optimize metal-support interactions (MSIs), providing suitable active sites for C-H activation. Meanwhile, the interfacial reactant spillover facilitates the further decomposition of activated intermediates. Thus, rationally exploiting interfacial effects is critical to enhancing catalytic activity. In this review, we analyzed recent advances in the following aspects: I. Understanding of the interface effects and design; II. Optimization of the catalyst-reactant contact, metal-support interface, and MSIs; III. Design of the interfacial composition and perimeter. Based on the analysis of the advances and current status, we provided challenges and opportunities for the rational design of interface nanostructures and interface-related stability. Meanwhile, a critical outlook was given on the interfacial sites of single-atom catalysts (SACs) for specific activation and catalytic selectivity.

Coupled anaerobic methane oxidation and metal reduction in soil under elevated CO2.

Continued current emissions of carbon dioxide (CO2 ) and methane (CH4 ) by human activities will increase global atmospheric CO2 and CH4 concentrations and surface temperature significantly. Fields of paddy rice, the most important form of anthropogenic wetlands, account for about 9% of anthropogenic sources of CH4 . Elevated atmospheric CO2 may enhance CH4 production in rice paddies, potentially reinforcing the increase in atmospheric CH4 . However, what is not known is whether and how elevated CO2 influences CH4 consumption under anoxic soil conditions in rice paddies, as the net emission of CH4 is a balance of methanogenesis and methanotrophy. In this study, we used a long-term free-air CO2 enrichment experiment to examine the impact of elevated CO2 on the transformation of CH4 in a paddy rice agroecosystem. We demonstrate that elevated CO2 substantially increased anaerobic oxidation of methane (AOM) coupled to manganese and/or iron oxides reduction in the calcareous paddy soil. We further show that elevated CO2 may stimulate the growth and metabolism of Candidatus Methanoperedens nitroreducens, which is actively involved in catalyzing AOM when coupled to metal reduction, mainly through enhancing the availability of soil CH4 . These findings suggest that a thorough evaluation of climate-carbon cycle feedbacks may need to consider the coupling of methane and metal cycles in natural and agricultural wetlands under future climate change scenarios.

Adhesive cryogel particles for bridging confined and irregular tissue defects.

BACKGROUND: Reconstruction of damaged tissues requires both surface hemostasis and tissue bridging. Tissues with damage resulting from physical trauma or surgical treatments may have arbitrary surface topographies, making tissue bridging challenging. METHODS: This study proposes a tissue adhesive in the form of adhesive cryogel particles (ACPs) made from chitosan, acrylic acid, 1-Ethyl-3-(3-dimethylaminopropyl) carbodiimide (EDC) and N-hydroxysuccinimide (NHS). The adhesion performance was examined by the 180-degree peel test to a collection of tissues including porcine heart, intestine, liver, muscle, and stomach. Cytotoxicity of ACPs was evaluated by cell proliferation of human normal liver cells (LO2) and human intestinal epithelial cells (Caco-2). The degree of inflammation and biodegradability were examined in dorsal subcutaneous rat models. The ability of ACPs to bridge irregular tissue defects was assessed using porcine heart, liver, and kidney as the ex vivo models. Furthermore, a model of repairing liver rupture in rats and an intestinal anastomosis in rabbits were established to verify the effectiveness, biocompatibility, and applicability in clinical surgery. RESULTS: ACPs are applicable to confined and irregular tissue defects, such as deep herringbone grooves in the parenchyma organs and annular sections in the cavernous organs. ACPs formed tough adhesion between tissues [(670.9 ± 50.1) J/m2 for the heart, (607.6 ± 30.0) J/m2 for the intestine, (473.7 ± 37.0) J/m2 for the liver, (186.1 ± 13.3) J/m2 for muscle, and (579.3 ± 32.3) J/m2 for the stomach]. ACPs showed considerable cytocompatibility in vitro study, with a high level of cell viability for 3 d [(98.8 ± 1.2) % for LO2 and (98.3 ± 1.6) % for Caco-2]. It has comparable inflammation repair in a ruptured rat liver (P = 0.58 compared with suture closure), the same with intestinal anastomosis in rabbits (P = 0.40 compared with suture anastomosis). Additionally, ACPs-based intestinal anastomosis (less than 30 s) was remarkably faster than the conventional suturing process (more than 10 min). When ACPs degrade after surgery, the tissues heal across the adhesion interface. CONCLUSIONS: ACPs are promising as the adhesive for clinical operations and battlefield rescue, with the capability to bridge irregular tissue defects rapidly.

Screening ionic liquids for efficiently extracting perfluoroalkyl chemicals (PFACs) from wastewater.

Liquid-liquid extraction (LLE) using ionic liquids (ILs)-based methods to remove perfluoroalkyl chemicals (PFACs), such as perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS), from wastewater, is an important strategy. However, the lack of physicochemical and LLE data limits the selection of the most suitable ILs for the extraction of PFACs. In this work, 1763 ILs for PFACs extraction from water were systematically screened using COSMOtherm to estimate the infinite dilution activity coefficient (lnγ∞)of PFOA and PFOS in water and ILs. To evaluate the accuracy of COSMOtherm, 8 ILs with various lnγ∞ values were selected, and their extraction efficiency (E) and distribution coefficient (Dexp) were measured experimentally. The results showed that the predicted lnγ∞ decreased as the increase of experimental extraction efficiency of PFOA or PFOS, while the tendency of predicted distribution coefficient (Dpre) was consistent with the experimental (Dexp) results. This work provides an efficient basis for selecting ILs for the extraction of PFACs from wastewater.

Robust adaptive super-twisting sliding mode formation controller for homing of multi-underactuated AUV recovery system with uncertainties.

This paper is concerned with the homing process in which a multi-underactuated AUV recovery system tracks the moving mother submarine in finite time in the presence of uncertain hydrodynamic parameters and unknown environmental disturbances. In the homing stage, underactuated AUVs and the moving mother submarine are treated as followers and the leader, respectively. The multi-underactuated AUV system finite time homing problem is converted to the leader-following finite-time formation control problem. The proposed leader-following formation strategy requires only the position information of the leader. The velocity of the leader can be designed as an additional degrees of freedom to stabilize position errors of the formation. A novel robust adaptive super-twisting sliding mode formation controller (ASTASMC) is proposed, specifically the super-twisting algorithm (STA) with adaptive uncertainty estimation. Wherein, the robust adaptive law can compensate for uncertainty with unknown upper bound in real time. Therefore, the proposed controller can not only enhance the tracking accuracy but also reduce the chattering. In addition, the finite-time convergence of estimation errors and tracking errors is rigorously proved. Finally, simulation results demonstrate the effectiveness of theoretical results.

Factors influencing fake news rebuttal acceptance during the COVID-19 pandemic and the moderating effect of cognitive ability.

Fake news is spreading rapidly on social media and poses a serious threat to the COVID-19 outbreak response. This study thus aims to reveal the factors influencing the acceptance of fake news rebuttals on Sina Weibo. Drawing on the elaboration likelihood model (ELM), we used text mining and the econometrics method to investigate the relationships among the central route (rebuttal's information readability and argument quality), peripheral route (rebuttal's source credibility, including authority and influence), and rebuttal acceptance, as well as the moderating effect of receiver's cognitive ability on these relationships. Our findings suggest that source authority had a negative effect on rebuttal acceptance, while source influence had a positive effect. Second, both information readability and argument quality had positive effects on rebuttal acceptance. In addition, individuals with low cognitive abilities relied more on source credibility and argument quality to accept rebuttals, while individuals with high cognitive abilities relied more on information readability. This study can provide decision support for practitioners to establish more effective fake news rebuttal strategies; it is especially valuable to reduce the negative impact of fake news related to major public health emergencies and safeguard the implementation of anti-epidemic strategies.

Extraction of PFOA from dilute wastewater using ionic liquids that are dissolved in N-octanol.

Polyfluoroalkyl Substances (PFAS) such as perfluorooctanoic acid (PFOA) are resistant to biodegradation leading to adverse health outcomes. Therefore, PFAS removal from drinking water is paramount. Liquid-liquid extraction processes can remove them from water; however, the hydrophobic and oleophobic properties of PFOA lead to the low extraction efficiency and severe emulsification, especially for the ppm-levels concentration of PFOA. Therefore, we introduced ionic liquid (IL) methyltrioctylammonium bis(trifluoromethylsulfonyl)imide ([A336][NTf2]) as extractant into octanol. We found that using hexadecyl trimethyl ammonium bromide (CTAB) as an extractant caused severe and stable emulsion. In comparison, [A336][NTf2] could suppress the emulsification with high extraction efficiency. The extraction performance of PFOA was examined as a function of various parameters. The results showed that the extraction efficiency was strongly dependent on the concentration of IL and aqueous pH. Further research revealed the extraction mechanisms at the molecular-level, and density functional theory (DFT) and molecular dynamic (MD) simulation agreed with the trends in the experiment. We determined that the extraction efficiency of PFOA from water could be up to 88.21 wt% for the optimized condition, indicating that the extraction system of [A336][NTf2] + octanol was efficient for separating PFOA from the diluted aqueous solution.

Large losses of ammonium-nitrogen from a rice ecosystem under elevated CO2.

Inputs of nitrogen into terrestrial ecosystems, mainly via the use of ammonium-based fertilizers in agroecosystems, are enormous, but the fate of this nitrogen under elevated atmospheric carbon dioxide (CO2) is not well understood. We have taken advantage of a 15-year free-air CO2 enrichment study to investigate the influence of elevated CO2 on the transformation of ammonium-nitrogen in a rice ecosystem in which ammonium is usually assumed to be stable under anaerobic conditions. We demonstrate that elevated CO2 causes substantial losses of ammonium-nitrogen that result from anaerobic oxidation of ammonium coupled to reduction of iron. We identify a new autotrophic member of the bacterial order Burkholderiales that may use soil CO2 as a carbon source to couple anaerobic ammonium oxidation and iron reduction. These findings offer insight into the coupled cycles of nitrogen and iron in terrestrial ecosystems and raise questions about the loss of ammonium-nitrogen from arable soils under future climate-change scenarios.

Development of a Three-Dimensional Electrochemical System Using a Blue TiO2/SnO2-Sb2O3 Anode for Treating Low-Ionic-Strength Wastewater.

Reducing energy use is crucial to commercialize electrochemical oxidation technologies. We developed a three-dimensional (3-D) electrochemical system that can significantly reduce the applied voltage and effectively degrade organic contaminants in low-ionic-strength wastewaters. The 3-D system consisted of a composite wire mesh anode (composed of blue TiO2 nanotubes covered with SnO2-Sb2O3), a proton exchange membrane, and a stainless-steel wire mesh cathode, which were compressed firmly together. For the 3-D system, we placed the anode of a 3-D electrode toward the wastewater that flowed past the anode. Both the two-dimensional (2-D) and 3-D systems had the same anode and cathode. We found that the 3-D system could reduce the applied voltage by 75.7% and reduce the electrical efficiency per log order reduction (EE/O) by 73% for 0.001 M Na2SO4. For Na2SO4 concentrations greater than 0.05 M, the 2-D system had a slightly lower EE/O. We also compared the EE/O of electrochemical advanced oxidation processes (EAOPs) with that of other advanced oxidation processes (UV/H2O2, UV/persulfate, O3/H2O2, UV/ TiO2, and UV/chlorine). We found that EAOPs have a much higher EE/O for low BA concentrations (20 mg/L) and a much lower EE/O for high BA concentrations (2000 mg/L).

Extreme rainfall trends of 21 typical urban areas in China during 1998-2015 based on remotely sensed data sets.

With the increase of population, many cities are growing in size at a phenomenal rate. Urbanization changes the urban underlying surface, influences the micro-climate, and sometimes affects the local precipitation process. In this study, we investigated the trends of extreme rainfall in China's 21 typical urban areas. Based on a series of daily rainfall and "Urban/built-up" dataset from TMPA 3B42 and MCD12Q1 products in China, trends in extreme precipitation, with the threshold defined as 95th (pre95p) and 99th (pre99p) percentiles of annual rain days during 1998-2015, have been assessed in China, and especially in 21 typical urban areas from 1998 to 2015. The tendency curves in extreme rainfall of different years are presented. In this period, more than 66% regions of China covered by TMPA 3B42 have increasing trends in extreme rainfall with pre95p threshold. The 21 typical urban areas showed different trends-in over half of these areas, upward tendencies in extreme rainfall were observed, particularly in Dalian, Beijing, and Chongqing. Seventeen urban areas showed increasing tendencies in pre95p extreme rainfall days, including Shanghai, Nanjing, Hangzhou, and Suzhou in the Yangtze River Delta region. The results also illustrate that southeastern coastal urban areas of China may have experienced decreasing occurrences in extreme rainfall.

Deactivation Mechanism of Multipoisons in Cement Furnace Flue Gas on Selective Catalytic Reduction Catalysts.

Increasing numbers of cement furnaces have applied selective catalytic reduction (SCR) units for advanced treatment of NO in the flue gas. However, the SCR catalysts may face various poisons, such as acidic, alkaline, and heavy metal species, in the fly ash. In this work, we studied the deactivation mechanisms of multipoisons (Ca, Pb, and S) on the CeO2-WO3/TiO2 catalyst, using the in situ diffuse reflectance infrared Fourier transform spectroscopy method. Calcium promoted the conversion of Ce(III) to Ce(IV) and, thus, (i) suppressed the redox cycle, (ii) decreased the NO adsorption (monodentate NO3- and bridged NO2-), and (iii) enriched the Lewis acid sites. Pb(IV) blocked Ce2(WO4)3, aggravating the electronegativity of W6+, which inhibited (i) the binding stability of tungsten and ammonia species, (ii) bridged NO3- (bonded to tungsten), and (iii) the Brønsted acid sites. The multipoisoning processes enriched O2- by repairing partial surface oxygen defects, which suppressed O22- and O-. Sulfur occupied the surface base sites and formed PbSO4 after Ce2(WO4)3 was saturated.

Comment on "The whole-soil carbon flux in response to warming".

In a compelling study, Hicks Pries et al (Reports, 31 March 2017, p. 1420) showed that 4°C warming enhanced soil CO2 production in the 1-meter soil profile, with all soil depths displaying similar temperature sensitivity (Q10). We argue that some caveats can be identified in their experimental approach and analysis, and that these critically undermine their conclusions and hence their claim that the strength of feedback between the whole-soil carbon and climate has been underestimated in terrestrial models.

Building Organic/Inorganic Hybrid Interphases for Fast Interfacial Transport in Rechargeable Metal Batteries.

We report a facile in situ synthesis that utilizes readily accessible SiCl4 cross-linking chemistry to create durable hybrid solid-electrolyte interphases (SEIs) on metal anodes. Such hybrid SEIs composed of Si-interlinked OOCOR molecules that host LiCl salt exhibit fast charge-transfer kinetics and as much as five-times higher exchange current densities, in comparison to their spontaneously formed analogues. Electrochemical analysis and direct optical visualization of Li and Na deposition in symmetric Li/Li and Na/Na cells show that the hybrid SEI provides excellent morphological control at high current densities (3-5 mA cm-2 ) for Li and even for notoriously unstable Na metal anodes. The fast interfacial transport attributes of the SEI are also found to be beneficial for Li-S cells and stable electrochemical cycling was achieved in galvanostatic studies at rates as high as 2 C. Our work therefore provides a promising approach towards rational design of multifunctional, elastic SEIs that overcome the most serious limitations of spontaneously formed interphases on high-capacity metal anodes.

Electrochemical Interphases for High-Energy Storage Using Reactive Metal Anodes.

Stable electrochemical interphases play a critical role in regulating transport of mass and charge in all electrochemical energy storage (EES) systems. In state-of-the-art rechargeable lithium ion batteries, they are rarely formed by design but instead spontaneously emerge from electrochemical degradation of electrolyte and electrode components. High-energy secondary batteries that utilize reactive metal anodes (e.g., Li, Na, Si, Sn, Al) to store large amounts of charge by alloying and/or electrodeposition reactions introduce fundamental challenges that require rational design in order to stabilize the interphases. Chemical instability of the electrodes in contact with electrolytes, morphological instability of the metal-electrolyte interface upon plating and stripping, and hydrodynamic-instability-induced electroconvection of the electrolyte at high currents are all known to cause metal electrode-electrolyte interfaces to continuously evolve in morphology, uniformity, and composition. Additionally, metal anodes undergo large changes in volume during lithiation and delithiation, which means that even in the rare cases where spontaneously formed solid electrode-electrolyte interphases (SEIs) are in thermodynamic equilibrium with the electrode, the SEI is under dynamic strain, which inevitably leads to cracking and/or rupture during extended battery cycling. There is an urgent need for interphases that are able to overcome each of these sources of instability with minimal losses of electrolyte and electrode components. Complementary chemical synthesis strategies are likewise urgently needed to create self-limited and mechanically durable SEIs that are able to flex and shrink to accommodate volume change. These needs are acute for practically relevant cells that cannot utilize large excesses of anode and electrolyte as employed in proof-of-concept-type experiments reported in the scientific literature. This disconnect between practical needs and research practices makes it difficult to translate promising literature results, underscoring the importance of research designed to reveal principles for good interphase design. This Account considers the fundamental processes involved in interphase formation, stability, and failure and on that basis identifies design principles, synthesis procedures, and characterization methods for enabling stable metal anode-electrolyte interfaces for EES. We first review results from experimental, continuum theoretical, and computational analyses of interfacial transport to identify fundamental connections between the composition of the SEI at metal-electrolyte interfaces and stability. Design principles and tools for creating stable artificial solid-electrolyte interphases (ASEIs) based on polymers, ionic liquids, ceramics, nanoparticles, salts, and their combinations are subsequently discussed. Interphases composed of a second electrochemically active material that stores charge by different processes from the underlying metal electrode emerge as particularly attractive routes toward so-called hybrid electrodes that enable facile scale-up of ASEI designs for commercially relevant EES.

LiF as an Artificial SEI Layer to Enhance the High-Temperature Cycle Performance of Li4Ti5O12.

Li4Ti5O12 (LTO) is a promising anode material for electric vehicles (EVs) and electrochemical energy storage applications because of its safety, good rate capability, and long cycle life. At elevated temperature, such as 60 °C, it always shows poor cycle performance because of the instability between the electrode material and electrolyte, which may also lead to a serious gassing issue. In this article, a facile hydrothermal method is adopted to coat the LTO powder with a thin LiF layer, in which the LiF acts as an artificial solid electrolyte interface (SEI) layer to prevent the direct contact of LTO and electrolyte, thus improving the high-temperature cycle performance. Electrochemical tests prove that the LiF coating layer has no influence on the kinetics at ambient temperature and greatly enhances the high-temperature cycle stability, and the LTO@LiF composite material keeps 87% of its initial discharge capacity in 300 1C cycles at 60 °C. Moreover, the LiF coating layer exhibits a special self-driven reforming process during the initial cycles, which makes it uniform and more effective at enhancing the stability between electrode/electrolyte interfaces.