Plasma-Activated Media Produced by a Microwave-Excited Atmospheric Pressure Plasma Jet Is Effective against Cisplatin-Resistant Human Bladder Cancer Cells In Vitro.

Media exposed to atmospheric pressure plasma (APP) produce reactive oxygen and nitrogen species (RONS), with hydrogen peroxide (H2O2), nitrite (NO2-), and nitrate (NO3-) being among the most detected species due to their relatively long lifetime. In this study, a standardized microwave-excited (ME) APP jet (APPJ) source was employed to produce gaseous RONS to treat liquid samples. The source was a commercially available plasma jet, which generated argon plasma utilizing a coaxial transmission line resonator at the operating frequency of 2.45 GHz. An ultraviolet-visible spectrophotometer was used to measure the concentrations of H2O2 and NO3- in plasma-activated media (PAM). Three different types of media (deionized water, Hank's balanced salt solution, and cell culture solution Dulbecco's modified eagles medium [DMEM]) were utilized as liquid samples. Among these media, the plasma-treated DMEM was observed to have the highest levels of H2O2 and NO3-. Subsequently, the feasibility of using argon ME-APPJ-activated DMEM (PAM) as an adjuvant to enhance the therapeutic effects of cisplatin on human bladder cancer cells (T-24) was investigated. Various cancer cell lines, including T-24 cells, treated with PAM were observed in vitro for changes in cell viability using the 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyl-2H-tetrazolium bromide (MTT) assay. A viability reduction was detected in the various cancer cells after incubation in PAM. Furthermore, the study's results revealed that PAM was effective against cisplatin-resistant T-24 cells in vitro. In addition, a possible connection between HER expression and cell viability was sketched.

Feature Selection Method Using Multi-Agent Reinforcement Learning Based on Guide Agents.

In this study, we propose a method to automatically find features from a dataset that are effective for classification or prediction, using a new method called multi-agent reinforcement learning and a guide agent. Each feature of the dataset has one of the main and guide agents, and these agents decide whether to select a feature. Main agents select the optimal features, and guide agents present the criteria for judging the main agents' actions. After obtaining the main and guide rewards for the features selected by the agents, the main agent that behaves differently from the guide agent updates their Q-values by calculating the learning reward delivered to the main agents. The behavior comparison helps the main agent decide whether its own behavior is correct, without using other algorithms. After performing this process for each episode, the features are finally selected. The feature selection method proposed in this study uses multiple agents, reducing the number of actions each agent can perform and finding optimal features effectively and quickly. Finally, comparative experimental results on multiple datasets show that the proposed method can select effective features for classification and increase classification accuracy.

Differential Sensitivity of Melanoma Cells and Their Non-Cancerous Counterpart to Cold Atmospheric Plasma-Induced Reactive Oxygen and Nitrogen Species.

Despite continuous progress in therapy, melanoma is one of the most aggressive and malignant human tumors, often relapsing and metastasizing to almost all organs. Cold atmospheric plasma (CAP) is a novel anticancer tool that utilizes abundant reactive oxygen and nitrogen species (RONS) being deposited on the target cells and tissues. CAP-induced differential effects between non-cancerous and cancer cells were comparatively examined. Melanoma and non-cancerous skin fibroblast cells (counterparts; both cell types were isolated from the same patient) were used for plasma-cell interactions. The production of intracellular RONS, such as nitric oxide (NO), hydroxyl radical (•OH), and hydrogen peroxide (H2O2), increased remarkably only in melanoma cancer cells. It was observed that cancer cells morphed from spread to round cell shapes after plasma exposure, suggesting that they were more affected than non-cancerous cells in the same plasma condition. Immediately after both cell types were treated with plasma, there were no differences in the amount of extracellular H2O2 production, while Hanks' balanced salt solution-containing cancer cells had lower concentrations of H2O2 than that of non-cancerous cells at 1 h after treatment. The melanoma cells seemed to respond to CAP treatment with a greater rise in RONS and a higher consumption rate of H2O2 than homologous non-cancerous cells. These results suggest that differential sensitivities of non-cancerous skin and melanoma cells to CAP-induced RONS can enable the applicability of CAP in anticancer therapy.

Coordinative Reduction of Metal Nodes Enhances the Hydrolytic Stability of a Paddlewheel Metal-Organic Framework.

Enhancement of hydrolytic stability of metal-organic frameworks (MOFs) is a challenging issue in MOF chemistry because most MOFs have shown limitations in their applications under a humid environment. Meanwhile, inner sphere electron transfer has constituted one of the most intensively studied subjects in contemporary chemistry. In this report, we show, for the first time, a new conceptual coordinative reduction of Cu2+ ion, which is realized in a paddlewheel MOF, HKUST-1, with a postsynthetic manner via inner sphere "single" electron transfer from hydroquinone (H2Q) to Cu2+ through its coordination bond. H2Q treatment of HKUST-1 under anhydrous conditions leads to the single charge (1+) reduction of approximately 30% of Cu2+ ions. Thus, this coordinative reduction is an excellent reduction process to be self-controlled in both oxidation state and quantity. As described below, once Cu2+ ions are reduced to Cu+, the reduction reaction does not proceed further, in terms of their oxidation state as well as their amount. Also, we demonstrate that a half of the Cu+ ions (about 15%) remains in paddlewheel framework with pseudo square planar geometry and the other half of the Cu+ ions (about 15%) forms [Cu(MeCN)4]+ complex in a small cage in the fashion of a ship-in-a-bottle after dissociation from the framework. Furthermore, we show that the coordinative reduction results in substantial enhancement of the hydrolytic stability of HKUST-1 to the extent that its structure remains intact even after exposure to humid air for two years.

Trapping of Stable [4n+1] π-Electron Species from Peripherally Substituted, Conformationally Rigid, Antiaromatic Hexaphyrins.

Peripherally substituted antiaromatic naphthorosarins have been synthesized for the first time. The synthesis was accomplished by acid-catalyzed condensation of naphthobipyrrole building blocks with aromatic aldehydes. The naphthobipyrrole building blocks were synthesized by simple oxidative coupling of the corresponding pyrrole substituted aromatics. Solid-state structural analyses of the synthesized naphthorosarins revealed that the presence of meso-2,6-dichlorophenyl- and 5,6-difluoro-substitution substantially alter the geometry and properties of the naphthorosarins. The substituents affect the redox potentials as well and, in turn, the proton-coupled electron-transfer processes leading to the formation of one- and two-electron reduced forms of the corresponding naphthorosarins. One particular naphthorosarin that bears both peripheral fluorine and meso-2,6-dichlorophenyl substituents forms a stable 25 π-electron species upon treating with TFA that was characterized by single-crystal X-ray diffraction analysis. The current study underscores how structural modifications can be used to fine-tune the electronic features of naphthorosarins, including stabilization of odd electron species.

A Chemical Role for Trichloromethane: Room-Temperature Removal of Coordinated Solvents from Open Metal Sites in the Copper-Based Metal-Organic Frameworks.

Open coordination sites (OCSs) in metal-organic frameworks (MOFs) have shown potential in applications such as molecular separation, sorption, catalysis, and sensing. Thus, the removal of coordinated solvent has been viewed as an essential step that needs to be performed prior to the use of the MOFs in the above applications. To date, a thermal method that is normally performed by applying heat and vacuum has been the most commonly employed activation method despite its negative influence on the structural integrity of the MOFs. In this report, we demonstrate that commonly inert trichloromethane (TCM) can activate OCSs; the TCM treatment process serves as an alternative chemical route to activation that does not require the external thermal energy. On the basis of the Raman study, we suggest a possible mechanism for the chemical activation process where TCM may weakly coordinate to the OCSs and then spontaneously dissociate. In addition, we prove that the chemical activation behavior is substantially boosted when a small amount of external heat energy (55 °C, 2.6 meV) is supplied during the TCM treatment. Using an HKUST-1-polyvinylidene fluoride (PVDF) mixed matrix (MM), we also demonstrate that this chemical activation strategy is a safe way to activate thermally deformable MOF-polymer mixed matrices.

Tailoring the Thermoelectric Properties of 3D-Printed n-Type Bi1.7Sb0.3Te3 with Incorporated Edge-Oxidized Graphene.

Using three-dimensional (3D) printing technology to fabricate Bi2Te3-based thermoelectric (TE) generators opens a potential way to create shape-conformable devices capable of recovering waste heat from thermal energy sources with diverse surface morphologies. However, pores formed in 3D-printed Bi2Te3-based materials by the removal of the organic ink binder result in unsatisfactory performance compared to the bulk materials, which has limited the widespread application of the ink-based 3D printing process. Furthermore, managing the volatile Se element in the n-type materials poses significant technological challenges compared to the p-type counterparts, resulting in a scarcity of research on 3D printing of n-type Bi2Te3. Here, we synthesized edge-oxidized graphene (EOG)-incorporated Se-free n-type Bi1.7Sb0.3Te3 (BST) using a direct ink writing (DIW) process with a binder-free novel ink. The incorporated EOG provides connectivity between small BST grains separated by pores and induces a bimodal-like grain structure during the DIW and sintering process. The optimal EOG content of 0.1 wt % in 3D-printed n-type BST simultaneously achieved both carrier transport control and active phonon scattering, due to its unique microstructure. A maximum ZT of 0.71 was obtained in the 0.1 wt % EOG/BST materials at 448 K, comparable to commercial bulk n-type Bi2Te3-based materials. Further, a single-element device composed of the EOG-BST material exhibited a 2-fold improvement in performance compared to pure-BST. These results open a technological route for the application of 3D printing technology for ink-based TE materials.

Synergistic Tailoring of Electronic and Thermal Transports in Thermoelectric Se-Free n-Type (Bi,Sb)2Te3.

Se-free n-type (Bi,Sb)2Te3 thermoelectric materials, outperforming traditional n-type Bi2(Te,Se)3, emerge as a compelling candidate for practical applications of recovering low-grade waste heat. A 100% improvement in the maximum ZT of n-type Bi1.7Sb0.3Te3 is demonstrated by using melt-spinning and excess Te-assisted transient liquid phase sintering (LPS). Te-rich sintering promotes the formation of intrinsic defects (TeBi), elevating the carrier concentration and enhancing the electrical conductivity. Melt-spinning with excess Te fine-tunes the electronic band, resulting in a high power-factor of 0.35 × 10-3 W·m-1 K-2 at 300 K. Rapid volume change during sintering induces the formation of dislocation networks, significantly suppressing the lattice thermal conductivity (0.4 W·m-1 K-1). The developed n-type legs achieve a high maximum ZT of 1.0 at 450 K resulting in a 70% improvement in the output power of the thermoelectric device (7.7 W at a temperature difference of 250 K). This work highlights the synergy between melt-spinning and transient LPS, advancing the tailored control of both electronic and thermal properties in thermoelectric technology.

Negative emotion can be "more negative" for those with high metacognitive abilities when problem-solving.

Introduction: Metacognitive monitoring ability enables you to learn and solve problems more efficiently through appropriate strategies. At the same time, those who are high in monitoring ability are known to allocate more cognitive resources to the perception and control of negative emotions, as compared to those with low metacognitive ability. Therefore, while monitoring emotions may help reduce the negative emotion by enabling efficient control, it could also interrupt the use of an efficient strategy when problem-solving, as cognitive resources may be depleted. Methods: To confirm this, we divided participants into groups with high and low monitoring abilities and manipulated emotions by presenting emotional videos. Subsequent to the manipulation, problem solving strategies were examined using items from the Cognitive Reflection Test (CRT). Results: Results showed that those who were high in monitoring ability were shown to use more efficient problem-solving strategies than those who were lower in monitoring ability, but only in situations when positive or no emotions were manipulated. However, as hypothesized, when negative emotion was aroused, the CRT scores of high monitoring ability group were significantly lowered, decreasing to the same performance as those with low monitoring ability. We also found that metacognitive monitoring ability, when interacting with emotion, indirectly affected CRT scores, and that monitoring and control, when affected by emotion, were mediated in the process. Discussion: These findings suggest a novel and complicated interaction between emotion and metacognition and warrant further research.

Isothermal Heteroepitaxy of Ge1-x Sn x Structures for Electronic and Photonic Applications.

Epitaxy of semiconductor-based quantum well structures is a challenging task since it requires precise control of the deposition at the submonolayer scale. In the case of Ge1-x Sn x alloys, the growth is particularly demanding since the lattice strain and the process temperature greatly impact the composition of the epitaxial layers. In this paper, the realization of high-quality pseudomorphic Ge1-x Sn x layers with Sn content ranging from 6 at. % up to 15 at. % using isothermal processes in an industry-compatible reduced-pressure chemical vapor deposition reactor is presented. The epitaxy of Ge1-x Sn x layers has been optimized for a standard process offering a high Sn concentration at a large process window. By varying the N2 carrier gas flow, isothermal heterostructure designs suitable for quantum transport and spintronic devices are obtained.

Crystalline hydrogen bonding of water molecules confined in a metal-organic framework.

Hydrogen bonding (H-bonding) of water molecules confined in nanopores is of particular interest because it is expected to exhibit chemical features different from bulk water molecules due to their interaction with the wall lining the pores. Herein, we show a crystalline behavior of H-bonded water molecules residing in the nanocages of a paddlewheel metal-organic framework, providing in situ and ex situ synchrotron single-crystal X-ray diffraction and Raman spectroscopy studies. The crystalline H-bond is demonstrated by proving the vibrational chain connectivity arising between hydrogen bond and paddlewheel Cu-Cu bond in sequentially connected Cu-Cu·····coordinating H2O·····H-bonded H2O and by proving the spatial ordering of H-bonded water molecules at room temperature, where they are anticipated to be disordered. Additionally, we show a substantial distortion of the paddlewheel Cu2+-centers that arises with water coordination simultaneously. Also, we suggest the dynamic coordination bond character of the H-bond of the confined water, by which an H-bond transitions to a coordination-bond at the Cu2+-center instantaneously after dissociating a previously coordinated H2O.

Neuropathological and behavioral features of an APP/PS1/MAPT (6xTg) transgenic model of Alzheimer's disease.

Alzheimer's disease is associated with various brain dysfunctions, including memory impairment, neuronal loss, astrocyte activation, amyloid-ß plaques, and neurofibrillary tangles. Transgenic animal models of Alzheimer's disease have proven to be invaluable for the basic research of Alzheimer's disease. However, Alzheimer's disease mouse models developed so far do not fully recapitulate the pathological and behavioral features reminiscent of Alzheimer's disease in humans. Here, we investigated the neurobehavioral sequelae in the novel 6xTg mouse model of Alzheimer's disease, which was developed by incorporating human tau containing P301L mutation in the widely used 5xFAD mouse model of Alzheimer's disease. At 11-months-old, 6xTg mice displayed the core pathological processes found in Alzheimer's disease, including accumulation of amyloid-ß plaque, extensive neuronal loss, elevated level of astrocyte activation, and abnormal tau phosphorylation in the brain. At 9 to 11-months-old, 6xTg mice exhibited both cognitive and non-cognitive behavioral impairments relevant to Alzheimer's disease, including memory loss, hyperlocomotion, anxiety-like behavior, depression-like behavior, and reduced sensorimotor gating. Our data suggest that the aged 6xTg mouse model of Alzheimer's disease presents pathological and cognitive-behavioral features reminiscent of Alzheimer's disease in humans. Thus, the 6xTg mouse model of Alzheimer's disease may be a valuable model for studying Alzheimer's disease-relevant non-cognitive behaviors.

Claustral MeCP2 Regulates Methamphetamine-induced Conditioned Place Preference in Cynomolgus Monkey.

The claustrum, a brain nucleus located between the cortex and the striatum, has recently been highlighted in drug-related reward processing. Methyl CpG-binding protein-2 (MeCP2) is a transcriptional regulator that represses or activates the expression of the target gene and has been known to have an important role in the regulation of drug addiction in the dopaminergic reward system. The claustrum is an important region for regulating reward processing where most neurons receive dopamine input; additionally, in this region, MeCP2 is also abundantly expressed. Therefore, here, we hypothesized that MeCP2 would be involved in drug addiction control in the Claustrum as well and investigated how claustral MeCP2 regulates drug addiction. To better understand the function of human claustral MeCP2, we established a non-human primate model of methamphetamine (METH) - induced conditioned place preference (CPP). After a habituation of two days and conditioning of ten days, the CPP test was conducted for three days. Interestingly, we confirmed that virus-mediated overexpression of MECP2 in the claustrum showed a significant reduction of METH-induced CPP in the three consecutive days during the testing period. Moreover, they showed a decrease in visit scores (frequency for visit) for the METH-paired room compared to the control group although the scores were statistically marginal. Taken together, we suggest that the claustrum is an important brain region associated with drug addiction, in which MeCP2 may function as a mediator in regulating the response to addictive drugs.

Prior failures, laboring in vain, and knowing when to give up: Incremental versus entity theories.

Against intuition, a set of "desirable difficulties" has been touted as a way in which to improve learning and lengthen retention. This includes, for instance, varying the conditions of learning to allow for more active, effortful, or challenging, contexts. In the current paper, we introduce data that show that, on the contrary, learning to know when to take the easy road may be crucial when it comes to avoiding "laboring in vain." We presented participants with prior problems - either easy or difficult - followed by choices of selecting an easy or a difficult current problem. Our primary goal was to examine the notion that past failures (which are more likely on the difficult prior items) may be a basis for allowing learners to then choose the easy rather than the difficult current problem. In other words, if one has labored in vain already, the easier items may now be more desirable. In addition, we compare the selections that are made between incremental and entity perspectives, given their fundamentally opposing views on effort. Our results showed that, interestingly, incremental theorists, who generally are proponents of effort, were more likely to select the easy problems, but only when they had experienced failure on prior, and similar, difficult tasks. We interpret these data to suggest that those holding an incremental view may be more in tune with their past efforts, resulting in a Metacognition-by-Experience, or ME strategy, and also hint at its generalizability through cross-cultural comparisons. Supplementary Information: The online version contains supplementary material available at 10.1007/s11409-020-09253-5.

A proteomic approach based on multiple parallel separation for the unambiguous identification of an antibody cognate antigen.

Autoantibodies obtained from cancer patients have been identified as useful tools for cancer diagnostics, prognostics, and as potential targets for immunotherapy. Serological proteome analysis in combination with 2-DE is a classic strategy for identification of tumor-associated antigens in the serum of cancer patients. However, serological proteome analysis cannot always indicate the true antigen out of a complex proteome identified from a single protein spot because the most abundant protein is not always the most antigenic. To address this problem, we utilized multiple parallel separation (MPS) for proteome separation. The common identities present in the fractions obtained using different separation methods were regarded as the true antigens. The merit of our MPS technique was validated using anti-ARPC2 and anti-PTEN antibodies. Next, we applied the MPS technique for the identification of glycyl-tRNA synthetase as the cognate antigen for an autoantibody that was overexpressed in the plasma of breast cancer patients. These results reveal that MPS can unambiguously identify an antibody cognate antigen by reducing false-positives. Therefore, MPS could be used for the characterization of diagnostic antibodies raised in laboratory animals as well as autoantibodies isolated from diseased patients.

Exploiting Microwave Chemistry for Activation of Metal-Organic Frameworks.

Microwave is thought of as a useful electromagnetic radiation tool because it is often used in real life as well as in a variety of chemical processes. Meanwhile, activation of metal-organic frameworks (MOFs), which must be essentially done to remove coordinating and pore-filling solvents before the use of MOFs for various applications, has been performed commonly with the methods of heat supply or solvent exchange. Here, we show a new methodological microwave activation (MA), realizing it with various MOFs such as HKUST-1, UiO-66, and MOF-74s. For instance, microwave irradiation to the MOF samples for 4-35 min leads to the complete activation of the MOFs without structural damage. As described below, we further demonstrate that the solvent-assisted MA, which is the MA process performed after the solvent exchange, can substantially reduce the time for the activation by 4 min.

Evaluation of murine norovirus, feline calicivirus, poliovirus, and MS2 as surrogates for human norovirus in a model of viral persistence in surface water and groundwater.

Human noroviruses (NoVs) are a significant cause of nonbacterial gastroenteritis worldwide, with contaminated drinking water a potential transmission route. The absence of a cell culture infectivity model for NoV necessitates the use of molecular methods and/or viral surrogate models amenable to cell culture to predict NoV inactivation. The NoV surrogates murine NoV (MNV), feline calicivirus (FCV), poliovirus (PV), and male-specific coliphage MS2, in conjunction with Norwalk virus (NV), were spiked into surface water samples (n = 9) and groundwater samples (n = 6). Viral persistence was monitored at 25 degrees C and 4 degrees C by periodically analyzing virus infectivity (for all surrogate viruses) and nucleic acid (NA) for all tested viruses. FCV infectivity reduction rates were significantly higher than those of the other surrogate viruses. Infectivity reduction rates were significantly higher than NA reduction rates at 25 degrees C (0.18 and 0.09 log(10)/day for FCV, 0.13 and 0.10 log(10)/day for PV, 0.12 and 0.06 log(10)/day for MS2, and 0.09 and 0.05 log(10)/day for MNV) but not significant at 4 degrees C. According to a multiple linear regression model, the NV NA reduction rates (0.04 +/- 0.01 log(10)/day) were not significantly different from the NA reduction rates of MS2 (0.05 +/- 0.03 log(10)/day) and MNV (0.04 +/- 0.03 log(10)/day) and were significantly different from those of FCV (0.08 +/- 0.03 log(10)/day) and PV (0.09 +/- 0.03 log(10)/day) at 25 degrees C. In conclusion, MNV shows great promise as a human NoV surrogate due to its genetic similarity and environmental stability. FCV was much less stable and thus questionable as an adequate surrogate for human NoVs in surface water and groundwater.

Interleukin-2 promotes angiogenesis by activation of Akt and increase of ROS.

Interleukin-2 plays a significant role in T cell proliferation. Here, we report the role of IL-2 in angiogenesis. IL-2 increased the ROS level and phosphorylation of Akt in human umbilical vein endothelial cells (HUVECs). IL-2 increased angiogenesis in an animal model and tube formation in HUVECs. The effect of IL-2 on angiogenesis and tube formation was mediated by ROS and Akt. This is the first report that IL-2 promotes angiogenesis.

Metal coordination and metal activation abilities of commonly unreactive chloromethanes toward metal-organic frameworks.

Over the last two decades, metal-organic frameworks (MOFs) have received particular attention because of their attractive properties such as permanent nanoporosity and the extraordinary functionality of open coordination sites (OCSs) at metal nodes. In particular, MOFs with open-state OCSs have shown potential in applications such as chemical separation, molecular sorption, catalysis, ionic conduction, and sensing. Thus, the activation of OCSs, i.e., the removal of coordinated solvent to produce open-state OCSs, has been viewed as an essential step that must be performed prior to the use of the MOFs in the aforementioned applications. This Feature Article focuses on the chemical functions of the commonly unreactive chloromethanes, i.e., dichloromethane (DCM) and trichloromethane (TCM), including their coordination to OCSs and activation of OCSs. Treatment with a chloromethane is a chemical route to activate OCSs that does not require an additional supply of external thermal energy. Importantly, a plausible mechanism for the chemical process, in which DCM and TCM weakly coordinate to the OCSs and then spontaneously dissociate in an intermediate step, which is proposed based on the results obtained from Raman studies will be discussed. Possible applications of chloromethane treatment to activate large-area MOF films and MOF-polymer mixed matrices, which can be propagated in molecular capture, will also be described.

Multiple Coordination Exchanges for Room-Temperature Activation of Open-Metal Sites in Metal-Organic Frameworks.

The activation of open coordination sites (OCSs) in metal-organic frameworks (MOFs), i.e., the removal of solvent molecules coordinated at the OCSs, is an essential step that is required prior to the use of MOFs in potential applications such as gas chemisorption, separation, and catalysis because OCSs often serve as key sites in these applications. Recently, we developed a "chemical activation" method involving dichloromethane (DCM) treatment at room temperature, which is considered to be a promising alternative to conventional thermal activation (TA), because it does not require the application of external thermal energy, thereby preserving the structural integrity of the MOFs. However, strongly coordinating solvents such as N,N-dimethylformamide (DMF), N,N-diethylformamide (DEF), and dimethyl sulfoxide (DMSO) are difficult to remove solely with the DCM treatment. In this report, we demonstrate a multiple coordination exchange (CE) process executed initially with acetonitrile (MeCN), methanol (MeOH), or ethanol (EtOH) and subsequently with DCM to achieve the complete activation of OCSs that possess strong extracoordination. Thus, this process can serve as an effective "chemical route" to activation at room temperature that does not require applying heat. To the best of our knowledge, no previous study has demonstrated the activation of OCSs using this multiple CE process, although MeOH and/or DCM has been popularly used in pretreatment steps prior to the TA process. Using MOF-74(Ni), we demonstrate that this multiple CE process can safely activate a thermally unstable MOF without inflicting structural damage. Furthermore, on the basis of in situ 1H nuclear magnetic resonance (1H NMR) and Raman studies, we propose a plausible mechanism for the activation behavior of multiple CE.