In this study, Mn-C composites using different MnO2 contents and solid carbon material were prepared to explore the synchronous removal performance of nutrients and SMX. Higher nitrate removal performance (97-98 %) with quickest nitrate removal rate (4.97 mg N L -1h- 1) was obtained in Mn\_20 systems. The increased Mn content and Mn-P compound were observed via surface characteristics, indicating the involvement of MnOx in pollutants removal, particularly for higher phosphorus removal (84-89 %) via Mn-P precipitation and BioMnOx adsorption. Nevertheless, compared to systems based on Mn\_0 composites (74 %), systems with Mn-C composites presented lower SMX reduction efficiency (34-51 %), which might be attributed to the large Mn(II) accumulation, impairing certain microbes and lower the MnOx function. Higher abundance of genera affiliated to Bacter-oidetes\_vadinHA17 and Rhodocyclaceae was observed in the Mn-C composites, as well as the gathering of Geo-bacter and Desulfovibrio as keystone taxa, responsible for the removal of nitrate and SMX and microbial interactions. Besides, the increase of sulfonamide ARGs was closely related to the predominant microbes in the Mn-C composites, which acted as the hosts of ARGs. This study broadens the knowledge of Mn-C composites in synergetic removal of nutrients and organics, and supports the potential application of manganese oxide in wastewater treatment.
The urban infrastructures of municipal solid waste (MSW) disposal play important roles in carbon reduction and building sustainable cities. China, with the world's largest MSW generation, has witnessed a relatively slow and spatially uneven transition progress of MSW disposal management. This study analysed the MSW disposal management transition and its determinants in Chinese cities of different sizes. Furthermore, the carbon reduction potential of MSW disposal management transition was estimated under different settings of policy reform. The results indicate that the MSW disposal management transition has made faster progress in cities with larger sizes, which could be ascribed to larger contradiction between city development and public service. The prediction results suggest that 73.13%–287.28% of carbon emission could be reduced by various policy reforms compared with the baseline scenario without policy intervention. Moreover, technological transformation should be specially underlined in mega cities, and household sorting should be specially underlined in medium cities.
As novel photocatalysts, covalent organic frameworks (COFs) have potential for water purification. Insufficient exciton dissociation and low charge mobility in COFs yet restricted their photocatalytic activity. Excitonic dissociation and charge transfer in COFs could be optimized via regulating the donor–acceptor (D–A) interactions through adjusting the number of donor units within COFs, yet relevant research is lacking. By integrating the 1,2,4-triazole or bis-1,2,4-triazole unit with quinone, we fabricated COF-DT (with a single donor unit) and COF-DBT (with double donor units) via a facile sonochemical method and used to decontaminate emerging contaminants. Due to the stronger D–A interactions than COF-DT, the exciton binding energy was lower for COF-DBT, facilitating the intermolecular charge transfer process. The degradation kinetics of tetracycline (model contaminant) by COF-DBT (k = (12.21 ± 1.29) × 10–2 min–1) was higher than that by COF-DT (k = (5.11 ± 0.59) × 10–2 min–1) under visible-light irradiation. COF-DBT could efficiently photodegrade tetracycline under complex water chemistry conditions and four real water samples. Moreover, six other emerging contaminants, both Gram-negative and Gram-positive strains, could also be effectively eliminated by COF-DBT. High tetracycline degradation performance achieved in a continuous-flow system and in five reused cycles in both laboratory and outdoor experiments with sunlight irradiation showed the stability and the potential for the practical application of COF-DBT.
With the developing technologies of artificial intelligence and the Internet of Things, intelligent IoT (iIoT) is prevailing currently. Design and implementation of integrated IoT nodes with continuous perception capability are indispensable to realize various smart terminal devices, which would also be vital to reduce the power consumption, improve the real-time performance, and enhance the security/privacy of the IoT system. In this paper, we present the architecture of “Sensing with Computing” and its chip design for smart sensing applications, which would support multi-modal perception signal processing with multi-dimension extension ability. Specially, we explore the analog/mixed-signal circuit designs and algorithm-hardware co-design methodologies for perception signal processing, and we also study the multi-modal integration of novel sensors and their interface technologies. Additionally, some multi-modal smart sensing systems with “Sensing + Computing in Memory” mixed-signal chips would be fabricated, which would support typical always-on smart sensing tasks.
Halogenated pharmaceuticals exhibit high toxicity if released to natural environment, and dehalogenation is a key process for their degradation. In this study, a reductive and directional dehalogenation technique, heterogenous formic acid (HCOOH) catalytic activation system, was proposed for diclofenac (DCF) dechlorination and detoxification. A functional material of Pd nanocluster decorated graphitic carbon nitride (Pd/g-C3N4) was developed for HCOOH activation. Although the optimized material (Pd1/g-C3N4) showed lower HCOOH decomposition rate (k1 = 0.287 ± 0.017 min−1) than the pristine Pd particles (k1 = 0.401 ± 0.031 min−1), it processed higher DCF degradation efficiency (97.9% within 30 min) than Pd particles. The enhancement mechanism was revealed by both experiments and theoretical calculations. Firstly, the six-fold cavities of g-C3N4 acted as anchor sites, which offered strong coordination environment for Pd nanoclusters. Secondly, the strong coordination environment of Pd led to upshifted d-band center of Pd 4d with enhanced bonding state, and then promoted HCOOH adsorption on Pd/g-C3N4, thus facilitating HCOOH decomposition through formate pathway rather than carboxyl pathway. Thirdly, Pd/g-C3N4 ensured HCOOH selectively decomposed as dehydrogenation reaction, which generated more H* (adsorbed H on Pd) than the dehydration reaction. The H* was proved to be the dominant reductive species for DCF hydrodechlorination. Moreover, the toxicities of DCF dechlorination products were greatly reduced.
Events are not isolated but rather linked to one another in various dimensions. In language processing, various sources of information—including real-world knowledge, (representations of) current linguistic input and non-linguistic visual context—help establish causal connections between events. In this review, we discuss causal inference in relation to events and event knowledge as one aspect of world knowledge, and their representations in language comprehension. To evaluate the mechanism and time course of causal inference, we gather insights from studies on (1) implicit causality/consequentiality as a specific form of causal inference regarding the protagonists of cause/consequence events, and (2) the processing of causal relations. We highlight the importance of methodology in measuring causal inference, compare the results from different research methods, and emphasize the contribution of the visual-world paradigm to achieve a better understanding of causal inference. We recommend that further investigations of causal inference consider temporally sensitive measures and more detailed contexts.
A series of C-doped Bi3O4X (X = Cl, Br, I) photocatalysts with layer-stacked structure was synthesized using glucose as carbon source, and the carbon doping and halogen species on harvesting broader solar spectrum and promoting charge carrier separation were systematically investigated. For pyrene photolysis, the photodegradation rate of pristine materials followed the order of Bi3O4I > Bi3O4Br > Bi3O4Cl, which was attributed to the difference in electronegativity of the halogen elements. The doped carbon boosted photocatalytic performance and the optimal C/Bi3O4I achieved 100% pyrene removal within 20 min, which primarily benefited from the dramatic improvement of the internal electric field (IEF). The improved IEF further increased the separation and transfer efficiency of photogenerated charge carriers. XRD and XPS characterizations confirmed that the doped carbon implanted into the lattice of [X] layers, and mainly affected the X np states. The X np orbitals contributed to the valence band (VB) of Bi3O4X, thus the local occupied states induced by doped carbon formed above VB and significantly decreased the VB potential. Meanwhile, the doped carbon narrowed the band gap and greatly improved visible light utilization. The O2−, h+ and OH were identified as dominant active species for pyrene degradation, and the generation rate of O2− and OH was further measured by the probe technique. Moreover, the photodegradation pathways of pyrene were proposed and the ecotoxicity of intermediates was assessed. This study reveals the effect of halogen species on photocatalytic activity and provides guidance for enhancing IEF by doping inorganic element.
A novel carbon quantum dots decorated C-doped α-Bi2O3 photocatalyst (CBO/CQDs) was synthesized by solvothermal method. The synergistic effect of adsorption and photocatalysis highly improved contaminants removal efficiencies. The ceftriaxone sodium degradation rate constant (k) of CBO/CQDs was 11.4 and 3.2 times that of pure α-Bi2O3 and C-doped α-Bi2O3, respectively. The interstitial carbon doping generated localized states above the valence band, which enhanced the utilization of visible light and facilitated the separation of photogenerated electrons and holes; the loading of CQDs improved the charge carrier separation and extended the visible light response; the reduced particle size of CBO/CQDs accelerated the migration of photogenerated carriers. The •O2− and h+ were identified as the dominant reactive species in ceftriaxone sodium degradation, and the key role of •O2− was further investigated by NBT transformation experiments. The Fukui index was applied to ascertain the molecular bonds of ceftriaxone sodium susceptible to radical attack, and intermediates analysis was conducted to explore the possible degradation pathways. The toxicity evaluation revealed that some degradation intermediates possessed high toxicity, thus the contaminants require sufficient mineralization to ensure safe discharge. The present study makes new insights into synchronous carbon dopping and CQDs decoration on modification of α-Bi2O3, which provides references for future studies.
Numerical resolution for 6-D Wigner dynamics under the Coulomb potential is faced with the combined challenges of high dimensionality, nonlocality, oscillation, and singularity. In particular, the extremely huge memory storage of 6-D grids hinders the usage of all existing deterministic numerical schemes, which is well known as the curse of dimensionality. To surmount these difficulties, we propose a massively parallel solver, termed the characteristic-spectral-mixed (CHASM) scheme, by fully exploiting two distinct features of the Wigner equation: locality of spatial advection and nonlocality of quantum interaction. Our scheme utilizes the local cubic B-spline basis to interpolate the local spatial advection. The key is to use a perfectly matched boundary condition to give a closure of spline coefficients, so that distributed pieces can recover the global one as accurately as possible owing to the rapid decay of wavelet basis in the dual space, and communication costs are significantly reduced. To resolve the nonlocal pseudodifferential operator with a singular symbol, CHASM further adopts the truncated kernel method to attain a highly efficient approximation. Several typical experiments including the quantum harmonic oscillator and the 1s state of hydrogen demonstrate the accuracy and efficiency of CHASM. Nonequilibrium electron-proton couplings are also clearly displayed and illuminate the uncertainty principle and quantum tunneling in phase space. Finally, the scalability of CHASM up to 16000 cores is presented.