Photothermal therapy (PTT) is one of the most promising approaches to combat multidrug‐resistant bacteria with less potential to induce resistance and systemic toxicity. However, uncontrollable ...distribution of photothermal agents leads to lethal temperatures for normal cells, and failure to offer timely and effective antibacterial stewardship. A pH switchable nanoplatform for persistent luminescence imaging‐guided precise PTT to selectively destroy only pathological cells while protecting nearby normal cells in bacterial infected microenvironment is shown. The PLNP@PANI‐GCS is fabricated by grafting polyaniline (PANI) and glycol chitosan (GCS) onto the surface of persistent luminescence nanoparticles (PLNPs). It takes advantage of the long persistent luminescence of PLNPs to realize autofluorescence‐free imaging, the pH‐dependent light–heat conversion property of PANI to get a stronger photothermal effect at pH 6.5 than pH 7.4, and the pH environment responsive surface charge transition of GCS. Consequently, PLNP@PANI‐GCS enables effective response to bacterial‐infected acid region and electrostatic bonding to bacteria in vivo, ensuring the spatial accuracy of near‐infrared light irradiation and specific heating directly to bacteria. In vivo imaging‐guided PTT to bacterial infection abscess shows effective treatment. PLNP@PANI‐GCS has great potential in treating multidrug‐resistant bacterial infection with low possibility of developing microbial drug resistance and little harm to normal cells.
A pH switchable nanoplatform is developed for in vivo persistent luminescent imaging and precise photothermal therapy of bacterial infections. This nanoplatform exhibits specific photothermal therapy to acidic bacterial‐infected regions but no damage to normal tissues.
Rainfall is considered as the dominant water replenishment in desert ecosystems, and the conversion of rainfall into soil water availability plays a central role in sustaining the ecosystem function. ...In this study, the role of biological soil crusts (BSCs), typically formed in the revegetated desert ecosystem in the Tengger Desert of China, in converting rainfall into soil water, especially for the underlying soil moisture dynamics, was clarified by taking into account the synthetic effects of BSCs, rainfall characteristics, and antecedent soil water content on natural rainfall conditions at point scale. Our results showed that BSCs retard the infiltration process due to its higher water holding capacity during the initial stage of infiltration, such negative effect could be offset by the initial wet condition of BSCs. The influence of BSCs on infiltration amount was dependent on rainfall regime and soil depth. BSCs promoted a higher infiltration through the way of prolonged water containing duration in the ground surface and exhibited a lower infiltration at deep soil layer, which were much more obvious under small and medium rainfall events for the BSCs area compared with the sand area. Generally, the higher infiltration at top soil layer only increased soil moisture at 0.03 m depth; in consequence, there was no water recharge for the deep soil, and thus, BSCs had a negative effect on soil water effectiveness, which may be a potential challenge for the sustainability of the local deep‐rooted vegetation under the site specific rainfall conditions in northwestern China.
Metal‐containing nanoparticles (M‐NPs) in metal/nitrogen‐doped carbon (M‐N‐C) catalysts have been considered hostile to the acidic oxygen reduction reaction (ORR). The relation between M‐NPs and the ...active sites of metal coordinated with nitrogen (MNx) is hard to establish in acid medium owing to the poor stability of M‐NPs. Herein, we develop a strategy to successfully construct a new FeCo‐N‐C catalyst containing highly active M‐NPs and MN4 composite sites (M/FeCo‐SAs‐N‐C). Enhanced catalytic activity and stability of M/FeCo‐SAs‐N‐C is shown experimentally. Calculations reveal that there is a strong interaction between M‐NPs and FeN4 sites, which can favor ORR by activating the O−O bond, thus facilitating a direct 4 e− process. Those findings firstly shed light on the highly active M‐NPs and FeN4 composite sites for catalyzing acid oxygen reduction reaction, and the relevant reaction mechanism is suggested.
Highly active metal‐containing nanoparticles and FeN4 composite sites have been constructed. Experiment and calculation results reveal the enormous potential for activating the O−O bond and promoting the direct 4 e− dissociation pathway in the acidic oxygen reduction reaction (ORR), which could fundamentally improve ORR activity and inhibit the formation of reactive oxygen species.
A facile anisotropic surface modification and etching strategy is presented for the synthesis of hollow structured ZIF‐67 nanoframes. The strategy uses structural and compositional distinctions ...between each crystallographic facet of truncated rhombic dodecahedrons ZIF‐67 (tZIF‐67 RDs) and the moderate coordinating and etching effects of cyanuric acid (CA). The CA can anisotropically modify and protect the {110} facets from etching, causing the six {100} facets be selectively etched via an inside‐out manner, and finally forming the hollow nanoframes. The surface‐modified hollow tZIF‐67 RDs can be facet‐selectively etched by metal salts in an outside‐in manner to give metal‐doped tZIF‐67 nanoframes. After calcination, the metal‐tZIF‐67 hybrids are converted into metal‐Co alloy/C composite catalysts with hollow nanoframed structures. The PtCo/C catalyst with only 5.9 wt % Pt exhibits high catalytic activities and stabilities in the hydrogen evolution reaction (HER) in acidic solutions.
CA molecules can anisotropically modify and protect the {110} facets of the tZIF‐67 crystal from etching, causing the six {100} facets be selectively etched via an inside‐out manner, and finally forming the hollow nanoframes. The surface modified hollow tZIF‐67 can further be facet‐selectively etched by metal salts in an outside‐in manner to give metal‐doped tZIF‐67 nanoframes.
•Three Neoproterozoic tectono-magmatic belts have been identified in South China.•An intra-oceanic arc and two active continental margins formed successively.•Their final collision welded the South ...China and yielded the Jiangnan Orogen.•In the end, the Jiangnan Orogen collapsed and the Nanhua rift basin formed.
According to the temporal-spatial distribution of Neoproterozoic igneous rocks and relative rocks in South China, including ophiolites, arc volcanic and intrusive rocks and subsequent bimodal magmatism, we identified the presence of a Neoproterozoic intra-oceanic arc, continent-arc-continent collision and three tectono-magmatic zones between the Yangtze Block and Cathaysia Block. We have also unraveled the amalgamation and tectono-magmatic histories between the Yangtze and Cathaysia blocks: At ∼1000–860Ma, northwestward ocean-ocean subduction and southeastward ocean-continent subduction resulted in the intra-oceanic arc magmatism and active continental margin magmatism in the Cathaysia Block respectively. At ∼860–825Ma, the steepening subduction caused development of back-arc basin in the intra-oceanic arc zone and the slab rollback induced the arc and back-arc magmatism in the Cathaysia Block. Meanwhile, a shallow dip northwestward ocean-continent subduction formed active continental margin magmatism in the Yangtze Block. At ∼825–805Ma, the continent-arc-continent collision and final amalgamation between the Yangtze and Cathaysia blocks yielded the Jiangnan Orogen. At ∼805–750Ma, the Jiangnan Orogen collapsed, and the Nanhua rift basin formed. Our study also rules out any Grenvillian Orogenic event and mantle plume activity in South China and indicates a marginal position of South China in the Rodinia supercontinent.
Enol ethers are widely used as quenching reagents for Grubbs catalysts. However, we report the surprisingly effective ring-opening metathesis polymerization (ROMP) of cyclic enol ethers, because the ...resulting electron-rich ruthenium alkylidene complex remains active toward metathesis of electron-rich olefins, despite its deactivation toward hydrocarbon olefins. We demonstrate the first example of ROMP of cyclic enol ethers, using 2,3-dihydrofuran as the monomer, producing a new type of degradable and depolymerizable poly(enol ether). The polymers exhibited perfect regioregularity, and their molecular weights can be regulated by the loading of Grubbs initiators or by the use of a linear vinyl ether as the chain transfer agent. We also developed protocols to deactivate the catalyst following metathesis of enol ethers and cleave the catalyst off the resulting polymers using H2O2 oxidation. The resulting poly(dihydrofuran) can be recycled to monomer via depolymerization with Grubbs catalyst or degraded to small molecules by hydrolysis under acidic conditions. This work opens exciting opportunities for a new class of ROMP monomers that lead to degradable polymers.
Extensive Late Mesozoic igneous rocks in SE China have been widely considered to be generated under the paleo-Pacific tectonic regime. Previous studies suggested a fundamental oceanward younging ...trend for the igneous rocks, further implying a NW-ward paleo-Pacific subduction model with gradual slab rollback. New LA–ICP–MS zircon U–Pb dating results show that early stage of the Late Mesozoic volcanic sequences (also known as the lower volcanic series) in Fujian Province was formed in three episodes: 160–148Ma for the Changlin Formation, 145–130Ma for the Nanyuan Formation, and 130–127Ma for the Xiaoxi Formation, among which the second episode made the volcanism climax. Thus the entire lower volcanic series in Fujian were formed earlier than those in Zhejiang (140–118Ma), displaying a NE-ward younging trend parallel to the potential subduction belt. Besides, in situ Hf isotope analyses on dated zircons yield an εHf(t) range of −19.2 to +1.7 for the lower volcanic series in Fujian. The majority of the studied volcanic rocks have more radiogenic Hf than that of the metamorphic basement, requiring the involvement of juvenile components in their origin. Moreover, the zircon εHf(t) value increases with time in each single area, as well as the igneous rocks elsewhere in SE China, except for the Changlin Formation which shows very opposite isotopic varying trend. Increasing zircon εHf(t) values imply an increasing material contribution of contemporaneous underplated mantle-derived magmas, which was plausibly induced by gradual crustal decompression. As well as the NE-ward younging trend of the lower volcanic series, it is also identified that the juvenile material contribution in the igneous petrogenesis gradually took place in the same direction along the coastal area. Thus here we propose an asynchronizing paleo-Pacific slab rollback model during 150–120Ma to account for the episodic magmatism and crustal extension in SE China. On the contrary, decreasing zircon εHf(t) values of the Changlin Formation volcanics indicate that they were formed under enhanced crustal compression probably induced by slab advance. On the other hand, the upper volcanic series in Fujian were formed during 110–88Ma coevally to those in Zhejiang, with more depleted zircon Hf isotopic compositions than the lower volcanic series as well, indicating that the entire coastal SE China was under the back-arc tectonic setting during that time.
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•J3–K1 volcanism in coastal SE China gradually took place from SW to NE.•We use extent of magma mixing to estimate the crustal extension or compression.•Late Mesozoic slab rollback beneath SE China is identified to be asynchronizing.
Driven by the persisting poor understanding of the sluggish kinetics of the hydrogen evolution reaction (HER) on Pt in alkaline media, a direct correlation of the interfacial water structure and ...activity is still yet to be established. Herein, using Pt and Pt–Ni nanoparticles we first demonstrate a strong dependence of the proton donor structure on the HER activity and pH. The structure of the first layer changes from the proton acceptors to the donors with increasing pH. In the base, the reactivity of the interfacial water varied its structure, and the activation energies of water dissociation increased in the sequence: the dangling O−H bonds < the trihedrally coordinated water < the tetrahedrally coordinated water. Moreover, optimizing the adsorption of H and OH intermediates can re‐orientate the interfacial water molecules with their H atoms pointing towards the electrode surface, thereby enhancing the kinetics of HER. Our results clarified the dynamic role of the water structure at the electrode–electrolyte interface during HER and the design of highly efficient HER catalysts.
On nickel–platinum alloy nanoparticles under alkaline conditions, the reactivity of interfacial water varies with its structure and the order of water dissociation. The inclusion of nickel re‐orientates interfacial water molecules with their hydrogen atoms pointing towards the electrode surface, thereby enhancing the kinetics of the hydrogen evolution reaction (HER).
The purpose of this paper is to analyze and research the practical activities of ideological and political education in colleges and universities using causal thinking design. Firstly, it studies the ...meaning and characteristics of ideological and political education and proposes a causal hypothesis. Secondly, the structural causal model is used to complete the basic structure of the causal thinking model, and the structural causal model is optimized using the HSIC Lasso method. Then, based on the Bayesian generative causal directional algorithm, the functional causal model is constructed, and the model is optimized. Based on the model, the Interaction Network Method for Civic Education Practice in Colleges and Universities is framed. Finally, based on the SCM algorithm, the learning effect of Civics in colleges and universities is analyzed. The
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and
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causal inference accuracy of the SCM algorithm is 100% and 90%, respectively. More than 70% of the students think that causal thinking exercises help to improve the learning effect of the Civics course.
Patients with locoregionally advanced nasopharyngeal carcinoma have a high risk of disease relapse, despite a high proportion of patients attaining complete clinical remission after receiving ...standard-of-care treatment (ie, definitive concurrent chemoradiotherapy with or without induction chemotherapy). Additional adjuvant therapies are needed to further reduce the risk of recurrence and death. However, the benefit of adjuvant chemotherapy for nasopharyngeal carcinoma remains controversial, highlighting the need for more effective adjuvant treatment options.
This multicentre, open-label, parallel-group, randomised, controlled, phase 3 trial was done at 14 hospitals in China. Patients (aged 18–65 years) with histologically confirmed, high-risk locoregionally advanced nasopharyngeal carcinoma (stage III–IVA, excluding T3–4N0 and T3N1 disease), no locoregional disease or distant metastasis after definitive chemoradiotherapy, an Eastern Cooperative Oncology Group performance status of 0 or 1, sufficient haematological, renal, and hepatic function, and who had received their final radiotherapy dose 12–16 weeks before randomisation, were randomly assigned (1:1) to receive either oral metronomic capecitabine (650 mg/m2 body surface area twice daily for 1 year; metronomic capecitabine group) or observation (standard therapy group). Randomisation was done with a computer-generated sequence (block size of four), stratified by trial centre and receipt of induction chemotherapy (yes or no). The primary endpoint was failure-free survival, defined as the time from randomisation to disease recurrence (distant metastasis or locoregional recurrence) or death due to any cause, in the intention-to-treat population. Safety was assessed in all patients who received at least one dose of capecitabine or who had commenced observation. This trial is registered with ClinicalTrials.gov, NCT02958111.
Between Jan 25, 2017, and Oct 25, 2018, 675 patients were screened, of whom 406 were enrolled and randomly assigned to the metronomic capecitabine group (n=204) or to the standard therapy group (n=202). After a median follow-up of 38 months (IQR 33–42), there were 29 (14%) events of recurrence or death in the metronomic capecitabine group and 53 (26%) events of recurrence or death in the standard therapy group. Failure-free survival at 3 years was significantly higher in the metronomic capecitabine group (85·3% 95% CI 80·4–90·6) than in the standard therapy group (75·7% 69·9–81·9), with a stratified hazard ratio of 0·50 (95% CI 0·32–0·79; p=0·0023). Grade 3 adverse events were reported in 35 (17%) of 201 patients in the metronomic capecitabine group and in 11 (6%) of 200 patients in the standard therapy group; hand-foot syndrome was the most common adverse event related to capecitabine (18 9% patients had grade 3 hand-foot syndrome). One (<1%) patient in the metronomic capecitabine group had grade 4 neutropenia. No treatment-related deaths were reported in either group.
The addition of metronomic adjuvant capecitabine to chemoradiotherapy significantly improved failure-free survival in patients with high-risk locoregionally advanced nasopharyngeal carcinoma, with a manageable safety profile. These results support a potential role for metronomic chemotherapy as an adjuvant therapy in the treatment of nasopharyngeal carcinoma.
The National Natural Science Foundation of China, the Key-Area Research and Development Program of Guangdong Province, the Natural Science Foundation of Guangdong Province, the Innovation Team Development Plan of the Ministry of Education, and the Overseas Expertise Introduction Project for Discipline Innovation.
For the Chinese translation of the abstract see Supplementary Materials section.