Single-Atom Fe-N4 Sites for Catalytic Ozonation to Selectively Induce a Nonradical Pathway toward Wastewater Purification.

Nonradical oxidation has been determined to be a promising pathway for the degradation of organic pollutants in heterogeneous catalytic ozonation (HCO). However, the bottlenecks are the rational design of catalysts to selectively induce nonradicals and the interpretation of detailed nonradical generation mechanisms. Herein, we propose a new HCO process based on single-atom iron catalysts, in which Fe-N4 sites anchored on the carbon skeleton exhibited outstanding catalytic ozonation activity and stability for the degradation of oxalic acid (OA) and p-hydroxybenzoic acid (pHBA) as well as the advanced treatment of a landfill leachate secondary effluent. Unlike traditional radical oxidation, nonradical pathways based on surface-adsorbed atomic oxygen (*Oad) and singlet oxygen (1O2) were identified. A substrate-dependent behavior was also observed. OA was adsorbed on the catalyst surface and mainly degraded by *Oad, while pHBA was mostly removed by O3 and 1O2 in the bulk solution. Density functional theory calculations and molecular dynamics simulations revealed that one terminal oxygen atom of ozone preferred bonding with the central iron atom of Fe-N4, subsequently inducing the cleavage of the O-O bond near the catalyst surface to produce *Oad and 1O2. These findings highlight the structural design of an ozone catalyst and an atomic-level understanding of the nonradical HCO process.

Enhanced Anaerobic Wastewater Treatment by a Binary Electroactive Material: Pseudocapacitance/Conductance-Mediated Microbial Interspecies Electron Transfer.

Anaerobic digestion (AD) is a promising method to treat organic matter. However, AD performance was limited by the inefficient electron transfer and metabolism imbalance between acid-producing bacteria and methanogens. In this study, a novel binary electroactive material (Fe3O4@biochar) with pseudocapacitance (1.4 F/g) and conductance (10.2 µS/cm) was exploited to store-release electrons as well as enhance the direct electron transfer between acid-producing bacteria and methanogens during the AD process. The mechanism of pseudocapacitance/conductance on mediating interspecies electron transfer was deeply studied at each stage of AD. In the hydrolysis acidification stage, the pseudocapacitance of Fe3O4@biochar acting as electron acceptors proceeded NADH/NAD+ transformation of bacteria to promote ATP synthesis by 21% which supported energy for organics decomposition. In the methanogenesis stage, the conductance of Fe3O4@biochar helped the microbes establish direct interspecies electron transfer (DIET) to increase the coenzyme F420 content by 66% and then improve methane production by 13%. In the complete AD experiment, electrons generated from acid-producing bacteria were rapidly transported to methanogens via conductors. Excess electrons were buffered by the pseudocapacitor and then gradually released to methanogens which alleviated the drastic drop in pH. These findings provided a strategy to enhance the electron transfer in anaerobic treatment as well as guided the design of electroactive materials.

The roles of time discounting and delay of gratification in career outcomes.

Although career development prominently features intertemporal choices (in which choice consequences play out over time), little is known about how an individual should navigate intertemporal career choices to obtain desirable career outcomes. Using a sample of U.S. workers (n = 340), the current study examined the structural predictions of two general intertemporal choice orientations (i.e., time discounting and delay of gratification) and one career-specific intertemporal choice orientation (i.e., career commitment) for career and life satisfaction. The results supported a sequential dual mediator model in which time discounting negatively predicts career and life satisfaction sequentially through delay of gratification and career commitment. Therefore, the present study supports the clinical utility of the intertemporal choice perspective in conceptualizing career fulfillment and facilitating career development and calls for more attention to the underrecognized intertemporal choice perspective in career research and practice. (PsycInfo Database Record (c) 2020 APA, all rights reserved).

Spatially-assembled binary carbon anode synergizing directional electron transfer and enriched microbe accommodation for wastewater treatment and energy conversion: From simulation to experiments.

Bioelectrochemical systems (BESs) hold prospects in wastewater energy and resource recovery. Anode optimization is important for simultaneous enhancement of wastewater energy conversion and effluent quality in BESs. In this study, a multi-physics model coupling fluid flow, organic degradation and electrochemical process was constructed to guide the design and optimization of BES anodes. Based on the multi-physics simulation, spatially-assembled binary carbon anodes composed of three-dimensional carbon mesh skeleton and granular activated carbon were proposed and established. The granular activated carbon conducive to microbe accommodation played a vital role in improving effluent water quality, while the carbon mesh skeleton favoring electron collection and transfer could enhance the bioelectricity output. With an average chemical oxygen demand (COD) removal rate of 0.442 kg m-3 d-1, a maximum power density of 20.6 W m-3 was achieved in the optimized composite anode BES, which was 25% and 154% higher than carbon mesh skeleton BES and granular activated carbon BES. Electroactive bacteria were enriched in composite anodes and performed important functions related to microbial metabolism and energy production. The spatially-assembled binary carbon anode with low carbon mesh packing density was more cost-effective with a daily energy output per anode cost of 221 J d-1 RMB-1. This study not only provides a cost-efficient alternative anode to simultaneously improve organic degradation and power generation performance, but also demonstrates the potential of multi-physics simulation in offering theoretical support and prediction for BES configuration design as well as optimization.

Mn-doped carbon-Al2SiO5 fibers enable catalytic ozonation for wastewater treatment: Interface modulation and mass transfer enhancement.

Heterogeneous catalytic ozonation is an efficient approach to remove hazardous and refractory organic contaminants in wastewater. It is crucial to design an ozone catalyst with high catalytic activity, high mass transfer and facile separation properties. Herein, easily separable aluminosilicate (Al2SiO5) fibers were developed as carriers and after interface modulation, Mn-doped carbon-Al2SiO5 (Mn-CAS) fibrous catalysts were proposed for catalytic ozonation. The growth of carbon shells on Al2SiO5 fiber surface and the introduction of metal Mn provided abundant Lewis acid sites to catalyze ozone. The Mn-CAS fiber/O3 system exhibited superior reactivity to degrade oxalic acid with a rate constant of 0.034 min-1, which was about 19 times as high as Al2SiO5/O3. For coal gasification wastewater treatment, Mn-CAS fibers also demonstrated high catalytic activity and stability and the COD removal was over 56%. Computational fluid dynamic simulations proved the high mass transfer properties of fibrous catalysts. Hydroxyl radicals (•OH) were identified as the predominant active species for organic degradation. Particularly, the catalytic pathways of O3 to •OH on Mn-O4 sites were revealed by theoretical calculations. This work provides a novel fibrous catalyst with high reactivity and mass transfer as well as easy separation characteristics for catalytic ozonation and wastewater purification.

Facile and low-cost ceramic fiber-based carbon-carbon composite for solar evaporation.

Solar-driven interfacial evaporation aiming at producing clean water without conventional energy consumption, has attracted worldwide research interest. Nevertheless, complex preparation processes and costly absorber materials might be the challenges for the practical application of this technology. Herein, a ceramic fiber was preferably selected as the supporting matrix, and a composite of activated carbon and carbon black was used as the photothermal material. Different evaporation system configurations containing the as-synthesized solar absorber were constructed and compared. It was found that, due to an improved heat insulation and water transportation, the one-dimensional configuration exhibited a maximum evaporation rate of 1.70 kg m-2 h-1 and the highest solar-to-vapor energy conversion efficiency of 91.8% under one sun. Furthermore, material cost and preparation complexity were also incorporated to assess the comprehensive performance of this solar absorber. The ceramic fiber-based activated carbon­carbon black composite (CF-ACB) solar absorber proposed in this contribution, featuring cost-effectiveness, easiness-to-manufacture and great evaporation performance, illuminated its application potential of future solar desalination to provide clean water for people who live in remote and less developed areas with limited and insufficient access to fresh water.