Antisolvent addition has been widely studied in crystallization in the pharmaceutical industries by breaking the solvation balance of the original solution. Here we report a similar antisolvent ...strategy to boost Zn reversibility via regulation of the electrolyte on a molecular level. By adding for example methanol into ZnSO4 electrolyte, the free water and coordinated water in Zn2+ solvation sheath gradually interact with the antisolvent, which minimizes water activity and weakens Zn2+ solvation. Concomitantly, dendrite‐free Zn deposition occurs via change in the deposition orientation, as evidenced by in situ optical microscopy. Zn reversibility is significantly boosted in antisolvent electrolyte of 50 % methanol by volume (Anti‐M‐50 %) even under harsh environments of −20 °C and 60 °C. Additionally, the suppressed side reactions and dendrite‐free Zn plating/stripping in Anti‐M‐50 % electrolyte significantly enhance performance of Zn/polyaniline coin and pouch cells. We demonstrate this low‐cost strategy can be readily generalized to other solvents, indicating its practical universality. Results will be of immediate interest and benefit to a range of researchers in electrochemistry and energy storage.
Water activity and Zn2+ solvation in an ZnSO4 electrolyte are regulated by adding methanol as antisolvent. Methanol gradually interacts with the free and coordinated water in the Zn2+ solvation sheath in the electrolyte, to suppress side reactions and enhance the Zn2+ transference number. Concomitantly, Zn2+ deposition orientation is changed, resulting in dendrite‐free Zn deposition and boosted Zn reversibility.
Zinc‐based electrochemistry is attracting significant attention for practical energy storage owing to its uniqueness in terms of low cost and high safety. However, the grid‐scale application is ...plagued by limited output voltage and inadequate energy density when compared with more conventional Li‐ion batteries. Herein, we propose a latent high‐voltage MnO2 electrolysis process in a conventional Zn‐ion battery, and report a new electrolytic Zn–MnO2 system, via enabled proton and electron dynamics, that maximizes the electrolysis process. Compared with other Zn‐based electrochemical devices, this new electrolytic Zn–MnO2 battery has a record‐high output voltage of 1.95 V and an imposing gravimetric capacity of about 570 mAh g−1, together with a record energy density of approximately 409 Wh kg−1 when both anode and cathode active materials are taken into consideration. The cost was conservatively estimated at <US$ 10 per kWh. This result opens a new opportunity for the development of Zn‐based batteries, and should be of immediate benefit for low‐cost practical energy storage and grid‐scale applications.
High‐voltage and scalable energy storage was demonstrated for a new electrolytic Zn–MnO2 battery system. Because of the new mechanism of two‐electron electrolysis/electrodeposition of Zn/Zn2+ and Mn4+/Mn2+, the system displayed a record‐high output voltage (1.95 V) and energy density (ca. 409 Wh kg−1). In addition, the electrolysis process was modeled by DFT calculations.
A promising new form-stable phase change material (PA/PB) was fabricated using pinecone biochar (PB) as the supporting material of palmitic acid (PA). The biochar of PB with large surface area was ...produced by forest residue of pinecone, and it was cheap, environment friendly and easy to prepare. The PB was firstly utilized as the supporter of PA and the characterizations of PA/PB were analyzed by the BET, SEM, XRD, DSC, TGA, FT-IR and thermal conductivity tester. The results demonstrated that the PA was physically absorbed by the PB and the crystal structure of the PA was not destroyed. The results of DSC showed that the fusing and crystallization points of the form-stable phase change material with the maximum content of PA (PA/PB-4) were 59.25 °C and 59.13 °C, and its fusing and freezing latent heat were 84.74 kJ/kg and 83.81 kJ/kg, respectively. The results of TGA suggested that the thermal stability of the PA/PB-4 composite was excellent, which could be used for the applications of thermal energy storage. Furthermore, the thermal conductivity of PA/PB-4 was 0.3926 W/(m∙K), which was increased by 43.76% compared with that of the pure PA. Thus, the study results indicated that the PA/PB-4 had great potential for thermal energy storage applications.
Improving the stability of sensitive catalytic systems is an emerging research topic in the catalysis field. However, the current design of heterogeneous catalysts mainly improves their catalytic ...performance. This paper presents a single‐atom catalyst (SAC) strategy to improve the cobalt‐catalysed fluorination of acyl chlorides. A stable Co−F intermediate can be formed through the oxidative fluorination of Co1−N4@NC SAC, which can replace the unstable high‐valent cobalt catalytic system and avoid the use of phosphine ligands. In the SAC system, KF can be employed as a fluorinating reagent to replace the AgF, which can be applied to various substrates and scale‐up conversion with high turnover numbers (TON=1.58×106). This work also shows that inorganic SACs have tremendous potential for organofluorine chemistry, and it provides a good reference for follow‐up studies on the structure‐activity relationship between catalyst design and chemical reaction mechanisms.
A Co single‐atom catalyst was synthesized via thermal decomposition of a zeolitic imidazolate framework (ZIF). The Co1−N4@NC catalyst generated a stable Co−F intermediate in situ through an oxidative fluorination pathway to replace the substitution fluorination of the unstable high‐valent Co system. In the presence of Co−F intermediates, KF can be used to replace AgF. Co1−N4@NC exhibited ultrahigh catalytic activity for the fluorination of acyl chlorides.
Alzheimer's disease (AD) is a growing concern in modern society, and effective drugs for its treatment are lacking.
(UR) and its main alkaloids have been studied to treat neurodegenerative diseases ...such as AD. This study aimed to uncover the key components and mechanism of the anti-AD effect of UR alkaloids through a network pharmacology approach. The analysis identified 10 alkaloids from UR based on HPLC that corresponded to 90 anti-AD targets. A potential alkaloid target-AD target network indicated that corynoxine, corynantheine, isorhynchophylline, dihydrocorynatheine, and isocorynoxeine are likely to become key components for AD treatment. KEGG pathway enrichment analysis revealed the Alzheimers disease (hsa05010) was the pathway most significantly enriched in alkaloids against AD. Further analysis revealed that 28 out of 90 targets were significantly correlated with Aβ and tau pathology. These targets were validated using a Gene Expression Omnibus (GEO) dataset. Molecular docking studies were carried out to verify the binding of corynoxine and corynantheine to core targets related to Aβ and tau pathology. In addition, the cholinergic synapse (hsa04725) and dopaminergic synapse (hsa04728) pathways were significantly enriched. Our findings indicate that UR alkaloids directly exert an AD treatment effect by acting on multiple pathological processes in AD.
From an operational point of view, several new entanglement detection criteria are proposed using quantum designs. These criteria are constructed by considering the correlations defined with quantum ...designs. Counter‐intuitively, the criteria with more settings are exactly equivalent to the corresponding ones with the minimal number of settings, namely the symmetric informationally complete positive operator‐valued measures (SIC POVMs). Fundamentally, this observation highlights the potentially unique role played by SIC POVMs in quantum information processing. Experimentally, this provides the minimal number of settings that one should choose for detecting entanglement. Furthermore, it is found that nonlinear criteria are not always better than linear ones for the task of entanglement detection.
By using quantum designs, this work explores the effects of the generalization of entanglement detection criteria based on symmetric informationally complete positive operator‐valued measures (SIC POVMs). Counter‐intuitively, no difference on the detection power is found between them. This highlights the unique role played by SIC POVMs in quantum information, meanwhile provides the minimal number of settings for experiments.
Advanced DNA synthesis, biosensor assembly, and genetic circuit development in synthetic biology and metabolic engineering have reinforced the application of filamentous bacteria, yeasts, and fungi ...as promising chassis cells for chemical production, but their industrial application remains a major challenge that needs to be solved.
As important chassis strains, filamentous microorganisms can synthesize important enzymes, chemicals, and niche pharmaceutical products through microbial fermentation. With the aid of metabolic engineering and synthetic biology, filamentous bacteria, yeasts, and fungi can be developed into efficient microbial cell factories through genome engineering, pathway engineering, tolerance engineering, and microbial engineering. Mutant screening and metabolic engineering can be used in filamentous bacteria, filamentous yeasts (Candida glabrata, Candida utilis), and filamentous fungi (Aspergillus sp., Rhizopus sp.) to greatly increase their capacity for chemical production. This review highlights the potential of using biotechnology to further develop filamentous bacteria, yeasts, and fungi as alternative chassis strains.
In this review, we recapitulate the recent progress in the application of filamentous bacteria, yeasts, and fungi as microbial cell factories. Furthermore, emphasis on metabolic engineering strategies involved in cellular tolerance, metabolic engineering, and screening are discussed. Finally, we offer an outlook on advanced techniques for the engineering of filamentous bacteria, yeasts, and fungi.
Lithium‐sulfur batteries hold promise for next‐generation batteries. A problem, however, is rapid capacity fading. Moreover, atomic‐level understanding of the chemical interaction between sulfur host ...and polysulfides is poorly elucidated from a theoretical perspective. Here, a two‐dimensional (2D) heterostructured MoN‐VN is fabricated and investigated as a new model sulfur host. Theoretical calculations indicate that electronic structure of MoN can be tailored by incorporation of V. This leads to enhanced polysulfides adsorption. Additionally, in situ synchrotron X‐ray diffraction and electrochemical measurements reveal effective regulation and utilization of the polysulfides in the MoN‐VN. The MoN‐VN‐based lithium‐sulfur batteries have a capacity of 708 mA h g−1 at 2 C and a capacity decay as low as 0.068 % per cycle during 500 cycles with sulfur loading of 3.0 mg cm−2.
V for victory: A two‐dimensional MoN‐VN heterostructure is investigated as a model sulfur host. The heterostructure can regulate polysulfides and improve sulfur utilization efficiency, resulting in superior rating and cycling performance. More importantly, incorporation of V in the heterostructure can effectively tailor the electronic structure of MoN, leading to enhanced polysulfides adsorption.
Lithium–sulfur batteries are a promising next‐generation energy storage device owing to their high theoretical capacity and the low cost and abundance of sulfur. However, the low conductivity and ...loss of active sulfur material during operation greatly limit the rating capabilities and cycling stability of lithium–sulfur batteries. In this work, a unique sulfur host hybrid material comprising nanosized nickel sulfide (NiS) uniformly distributed on 3D carbon hollow spheres (C‐HS) is fabricated using an in situ thermal reduction and sulfidation method. In the hybrid material, the nanosized NiS provides a high adsorption capability for polysulfides and the C‐HS serves as a physical confinement for polysulfides and also a 3D electron transfer pathway. Moreover, NiS has strong chemical coupling with the C‐HS, favoring fast charge transfer and redox kinetics of the sulfur electrode. With a sulfur loading of up to 2.3 mg cm−2, the hybrid material‐based lithium–sulfur batteries offer a capacity decay as low as 0.013% per cycle and a capacity of 695 mA h g−1 at 0.5 C after 300 cycles. This unique 3D hybrid material with strong chemical coupling provides a promising sulfur host for high performance lithium–sulfur batteries.
A unique 3D hybrid of nickel sulfide (NiS) and carbon hollow spheres (C‐HSs) is synthesized as a sulfur host. The uniformly distributed NiS greatly promote adsorption capability toward polysulfides.The C‐HSs increase sulfur loading as well as the overall conductivity. This sulfur host achieves a capacity of 695 mA h g−1 after 300 cycles at 0.5 C.
•We combine Zelinsky's hypothesis of the mobility transition model and land use transition theory to explore land use change.•We examine changes in rural out-migration and land use in China from a ...transition perspective.•Land use transition in China has unique characters, such as hollowed villages, because of institutional environment.•Deal with the food–environment-development trilemma, policies should consider the impact of rural out-migration on land use transition.
Although rural out-migration has significantly transformed land use at the local to regional scale, the links between rural out-migration and land use change are not well understood. This paper connects Zelinsky's mobility transition model to land use transition theory and identifies the impacts of rural out-migration on land use transition. It then explores the significant influences of rural out-migration on land use transition in China. Since the introduction of economic reforms in 1978, China has undergone rapid and significant changes. Extensive rural out-migration has transformed China from a land-attached agricultural society to an urban and industrial society. This has produced several contrasting land use trends: increased land demand in urban areas at the expense of high-quality cultivated land, increased number of total settlement areas and emerging “hollowed villages” in the countryside. China's policies addressing these problems could benefit to other developing countries, such as restricting frontier clearing through land zoning and other ecological protection policies; encouraging nonmigrants to adjust their agricultural land holdings; protecting nonmigrants’ interest through subsidizing agricultural land, and improving rural infrastructure and farmers’ living conditions. Rural out-migration is thus a critical element in addressing the fundamental question of land use—how to balance the land demand for economic development, food security and conservation. This article explores the impacts of rural out-migration on land use change, analyzes the process of migration and land use transition and then examines how rural out-migration affects land use transition in China. This paper also explores future land use change in China, by considering the trend of rural–urban migration and the dynamics of population transition. In so doing, we try to link current rural out-migration dynamics and land use change to facilitate future research and policy considerations. We propose that in order to facilitate policymaking, further research should take a multiscale perspective: cross-country research should be based on an understanding of the dynamics and issues of rural out-migration and land use change in developing countries with different characteristics; country-level research should focus on land use change and problems caused by rural out-migration and its spatial characteristics; and community and household-level research should examine the effects of out-migration of household or household members on agricultural and other land use change.
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