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1.
ChemSusChem ; : e202301449, 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38647354

RESUMO

Plastic wastes continuously accumulate, causing critical environmental issues. It is urgent to develop efficient strategies to convert them to valuable products. Very recently, two novel approaches for plastic recycling were reported by Huber et al. (Science, 2023, 381, 660-666) and Liu et al. (Science, 2023, 381, 666-671) , where polyethylene (PE) and polypropylene (PP) plastics were converted into potentially valuable products, such as alcohols, aldehydes, surfactants, and detergents. The two processes achieved complete degradation, high selectivity of target products, as well as high values of products, showing economic feasibility for industrial scale-up. These breakthroughs for plastic recycling are highlighted in this article.

2.
Small ; : e2311684, 2024 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-38533989

RESUMO

Carbonate-superstructured solid fuel cells (CSSFCs) are an emerging type of fuel cells with high flexibility of fuels. However, using ethane fuel for solid fuel cells is a great challenge due to serious degradation of their anodes. Herein, this critical issue is solved by creating a novel gradient functional layer anode for CSSFCs. First, a finer-scale anode with a larger surface area is demonstrated to provide more active sites for the internal reforming reaction of ethane, achieving a 60% higher ethane conversion rate and 40% lower polarization resistance than conventional anodes. Second, incorporating a gradient functional layer into the anode results in an additional 50% enhancement in the peak power density of CSSFCs to a record high value (up to 241 mW cm-2) with dry ethane fuel at a low temperature of 550 °C, which is even comparable to the power density of conventional solid oxide fuel cells above 700 °C. Furthermore, the CSSFC with the gradient anode exhibits excellent durability for over 200 h. This finding provides a new strategy to develop efficient anodes for hydrocarbon fuels.

3.
Proc Natl Acad Sci U S A ; 121(2): e2314996121, 2024 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-38165931

RESUMO

Converting hydrocarbons and greenhouse gases (i.e., carbon dioxide, CO2) directly into electricity through fuel cells at intermediate temperatures (450 to 550 °C) remains a significant challenge, primarily due to the sluggish activation of C-H and C=O bonds. Here, we demonstrated a unique strategy to address this issue, in which light illumination was introduced into the thermal catalytic CO2 reforming of ethane in the anode as a unique thermo-photo anode process for carbonate-superstructured solid fuel cells. The light-enhanced fuel activation led to excellent cell performance with a record-high peak power density of 168 mW cm-2 at an intermediate temperature of 550 °C. Furthermore, no degradation was observed during ~50 h operation. Such a successful integration of photo energy into the fuel cell system provides a new direction for the development of efficient fuel cells.

4.
J Phys Chem Lett ; 15(1): 142-147, 2024 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-38148277

RESUMO

As a distinct type of fuel cell, a carbonate-superstructured solid fuel cell (CSSFC), which possesses excellent performance and easy fabrication as well as low cost, was recently invented by our group. Herein, we demonstrated the critical role of the in-situ-generated eutectic carbonate phase in CSSFC. Namely, the in-situ generation of eutectic Li2CO3/Na2CO3 system increased the oxygen ionic conductivity of Ce0.8Sm0.2O1.9 solid electrolyte by 20 times (from 3.5 × 10-3 to 7.3 × 10-2 S cm-1), leading to 6 times enhancement of CSSFC peak powder density (up to 206 mW cm-2) with methane fuel at 550 °C. This finding is extremely important for designing efficient CSSFCs.

5.
Adv Sci (Weinh) ; : e2306132, 2023 Dec 03.
Artigo em Inglês | MEDLINE | ID: mdl-38044296

RESUMO

2D materials, such as graphene, MXenes (metal carbides and nitrides), graphdiyne (GDY), layered double hydroxides, and black phosphorus, are widely used as electrocatalyst supports for alcohol oxidation reactions (AORs) owing to their large surface area and unique 2D charge transport channels. Furthermore, the development of highly efficient electrocatalysts for AORs via tuning the structure of 2D support materials has recently become a hot area. This article provides a critical review on modification strategies to develop 2D material-based electrocatalysts for AOR. First, the principles and influencing factors of electrocatalytic oxidation of alcohols (such as methanol and ethanol) are introduced. Second, surface molecular functionalization, heteroatom doping, and composite hybridization are deeply discussed as the modification strategies to improve 2D material catalyst supports for AORs. Finally, the challenges and perspectives of 2D material-based electrocatalysts for AORs are outlined. This review will promote further efforts in the development of electrocatalysts for AORs.

6.
J Phys Chem Lett ; 14(47): 10710-10716, 2023 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-37988703

RESUMO

The van der Waals (vdW) assemblies are the most common structures of materials. However, direct mapping of intermolecular electron clouds of a vdW assembly has never been obtained, even though the intramolecular electron clouds were visualized by atomic-resolution techniques. In this report, we unprecedentedly mapped the intermolecular electron cloud of the assemblies of ethanol molecules via ethyl groups with high-resolution atomic force microscopy and scanning tunneling microscopy at 5 K, leading to the first visualization of vdW molecular chains, in which ethanol molecules assemble into twin vdW molecular chains in a reverse parallel configuration on the Ag(111) plane. Furthermore, spontaneous order-disorder transitions in the chain were dynamically observed, suggesting its unusual properties different from those of 2D vdW materials. These findings provide an "eye" to see the atomic world of vdW materials.

7.
Sci Total Environ ; 905: 167251, 2023 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-37741410

RESUMO

Plastics have been widely used in daily life and industries due to their low cost and high durability, leading to huge production of plastics and tens of millions of plastic wastes every year. Chemical recycling can recycle contaminated and degraded plastics (that mechanical recycling cannot deal with) to obtain value-added products, which potentially solves the environmental problems caused by plastics and realizes a circular economy. Alkaline earth metal oxides, as a category of cost-effective and multi-functional materials, have been widely used in chemical recycling of common plastics, acting as three roles: catalyst, template, and absorbent. Among five commercial plastics, polyethylene terephthalate is suitable for pyrolysis and solvolysis. Polyethylene and polypropylene, which are ideal precursors for synthesis of carbon nanotubes, could be combined with biomass for co-pyrolysis. Polyvinyl chloride needs to be pretreated to reduce chloride content prior to pyrolysis. Depolymerization of polystyrene into monomers is attractive. This review summarized the chemical recycling approaches of commercial plastics and the strategies with alkaline earth metal oxides for the development of efficient recycling processes. It will aid understanding of the advances and challenges in the field and promote the future research.

8.
Chemosphere ; 335: 139077, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37263507

RESUMO

The heavy metal pollution constitutes a critical environmental issue. This has stimulated intensive efforts to develop treatment techniques for their removal from wastewater, including adsorption, membrane separation, precipitation/electrodeposition, ion exchange, coagulation-flocculation, flotation/electroflotation, solvent extraction, catalysis, and bioremediation. This article provides a comprehensive review on the advances in those techniques with the focus on the recent decade (2013-2023). It shows that the adsorption has attracted the most attention and membrane filtration the second, followed by precipitation and ion exchange. Interests in bioremediation and electrochemical treatments as well as catalysis are expected to increase in the future. Furthermore, the combination of different processes is a promising strategy to develop efficient hybrid technologies.


Assuntos
Metais Pesados , Poluentes Químicos da Água , Purificação da Água , Águas Residuárias , Adsorção , Floculação , Troca Iônica , Poluentes Químicos da Água/análise , Purificação da Água/métodos
9.
Int J Mol Sci ; 24(10)2023 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-37240435

RESUMO

Antibiotic tolerance has become an increasingly serious crisis that has seriously threatened global public health. However, little is known about the exogenous factors that can trigger the development of antibiotic tolerance, both in vivo and in vitro. Herein, we found that the addition of citric acid, which is used in many fields, obviously weakened the bactericidal activity of antibiotics against various bacterial pathogens. This mechanistic study shows that citric acid activated the glyoxylate cycle by inhibiting ATP production in bacteria, reduced cell respiration levels, and inhibited the bacterial tricarboxylic acid cycle (TCA cycle). In addition, citric acid reduced the oxidative stress ability of bacteria, which led to an imbalance in the bacterial oxidation-antioxidant system. These effects together induced the bacteria to produce antibiotic tolerance. Surprisingly, the addition of succinic acid and xanthine could reverse the antibiotic tolerance induced by citric acid in vitro and in animal infection models. In conclusion, these findings provide new insights into the potential risks of citric acid usage and the relationship between antibiotic tolerance and bacterial metabolism.


Assuntos
Antibacterianos , Estresse Oxidativo , Animais , Antibacterianos/farmacologia , Bactérias , Ciclo do Ácido Cítrico
10.
Chem Commun (Camb) ; 59(48): 7383-7386, 2023 Jun 13.
Artigo em Inglês | MEDLINE | ID: mdl-37248993

RESUMO

The sp-hybridized carbon chain (carbyne) is a representative 1D atomic material, whose bonding structure and chemical reactivity have remained a mystery for a century. Here, we report the unexpected alternating bond orders of 1.4 and 2.6 for the most stable carbon chain and the in situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) detection of the temperature-dependent reversible change of the bond order alternation. Moreover, we revealed its reactivities with O2, H2, and CO2 at temperatures up to 600 °C and created an end-group-protection strategy to stabilize it. These observations open a new door to the chemistry of atomic materials.

11.
Chem Commun (Camb) ; 59(44): 6660-6673, 2023 May 30.
Artigo em Inglês | MEDLINE | ID: mdl-37144412

RESUMO

Three-dimensional (3D) graphene is one of the most important nanomaterials. This feature article highlights the advancements, with an emphasis on contributions from our group, in the synthesis of 3D graphene-based materials and their utilization in solar cells. Chemistries of graphene oxides, hydrocarbons, and alkali metals are discussed for the synthesis of 3D graphene materials. Their performances in dye-sensitized solar cells and perovskite solar cells (as counter electrodes, photoelectrodes, and electron extracting layers) were correlatively analyzed with their properties/structures (accessible surface area, electrical conductivity, defects, and functional groups). The challenges and prospects for their applications in photovoltaic solar cells are outlined.

12.
Nat Commun ; 14(1): 1203, 2023 03 02.
Artigo em Inglês | MEDLINE | ID: mdl-36864061

RESUMO

Large numbers of leaves fall on the earth each autumn. The current treatments of dead leaves mainly involve completely destroying the biocomponents, which causes considerable energy consumption and environmental issues. It remains a challenge to convert waste leaves into useful materials without breaking down their biocomponents. Here, we turn red maple dead leaves into an active three-component multifunctional material by exploiting the role of whewellite biomineral for binding lignin and cellulose. Owing to its intense optical absorption spanning the full solar spectrum and the heterogeneous architecture for effective charge separation, films of this material show high performance in solar water evaporation, photocatalytic hydrogen production, and photocatalytic degradation of antibiotics. Furthermore, it also acts as a bioplastic with high mechanical strength, high-temperature tolerance, and biodegradable features. These findings pave the way for the efficient utilization of waste biomass and innovations of advanced materials.


Assuntos
Celulose , Lignina , Biopolímeros , Antibacterianos , Biomassa
13.
World J Clin Cases ; 11(7): 1615-1626, 2023 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-36926400

RESUMO

BACKGROUND: Pacemaker lead-induced heart perforation is a rare but life-threatening complication of pacemaker implantation, and timely diagnosis remains a challenge for clinicians. Here, we report a case of pacemaker lead-induced cardiac perforation rapidly diagnosed by a "bow-and-arrow" sign on point-of-care ultrasound (POCUS). CASE SUMMARY: A 74-year-old Chinese woman who had undergone permanent pacemaker implantation 26 d before suddenly developed severe dyspnea, chest pain, and hypotension. The patient had received emergency laparotomy for an incarcerated groin hernia and was transferred to the intensive care unit 6 d before. Computed tomography was not available due to unstable hemodynamic status, so POCUS was performed at the bedside and revealed severe pericardial effusion and cardiac tamponade. Subsequent pericardiocentesis yielded a large volume of bloody pericardial fluid. Further POCUS by an ultrasonographist revealed a unique "bow-and-arrow" sign indicating right ventricular (RV) apex perforation by the pacemaker lead, which facilitated the rapid diagnosis of lead perforation. Given the persistent drainage of pericardial bleeding, urgent off-pump open chest surgery was performed to repair the perforation. However, the patient died of shock and multiple organ dysfunction syndrome within 24 h post-surgery. In addition, we also performed a literature review on the sonographic features of RV apex perforation by lead. CONCLUSION: POCUS enables the early diagnosis of pacemaker lead perforation at the bedside. A step-wise ultrasonographic approach and the "bow-and-arrow" sign on POCUS are helpful for rapid diagnosis of lead perforation.

14.
Front Endocrinol (Lausanne) ; 14: 1134877, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36967788

RESUMO

Objectives: This work aimed to observe the effect of consuming Chinese herb tea on glucolipid metabolism and gut microbiota in patients with type 2 diabetes mellitus (T2DM). Methods: Ninety patients with T2DM were recruited from a community and randomly divided into the control group (CG) and intervention group (IG). CG maintained conventional treatment and lifestyle, and IG accepted additional "maccog" traditional Chinese medicine (TCM) tea (mulberry leaf, radix astragali, corn stigma, cortex lycii, radix ophiopogonis, and gynostemma) for 12 weeks. Glucolipid metabolism, hepatorenal function, and gut microbiota were then measured. Results: After the intervention, the decreases in fasting plasma glucose (FPG) and total cholesterol (TC) were greater (P<0.05) in IG than in CG, and those in glycosylated serum protein (GSP) were almost significantly greater (P=0.066) in IG than in CG. The total protein (TP), albumin (ALB), and creatinine (CREA) levels in IG were significantly lower and their decreases were larger in IG than in CG (P<0.05) after the intervention. The Ace and Chao1 indices in IG were slightly higher after the intervention (P=0.056 and 0.052, respectively) than at baselines. The abundance of Actinobacteria, Lachnospiraceae, Bifidobacteriaceae, and Phascolarctobacterium increased significantly after the intervention in IG (P<0.05), and the abundance was higher in IG than in CG (P<0.05 or P<0.1). The abundance of Clostridiales and Lactobacillales was negatively correlated with FPG (P<0.05), Clostridiales and Lachnospiraceae was negatively correlated with GSP (P<0.05), and Bacteroides/Firmicutes was positively correlated with both (P<0.05). No adverse event was observed during the intervention. Conclusions: Administration of "maccog" TCM tea for 12 weeks slightly improved glucolipid metabolism and significantly increased the abundance of beneficial gut microbiota in community patients with T2DM. The increase in beneficial bacteria abundance may be involved in the improvement of glucose metabolism indicators. In addition, this intervention is safe and feasible. Clinical trial registration: https://www.chictr.org.cn/showproj.aspx?proj=31281, identifier ChiCTR1800018566.


Assuntos
Actinobacteria , Diabetes Mellitus Tipo 2 , Microbioma Gastrointestinal , Humanos , Diabetes Mellitus Tipo 2/metabolismo , Medicina Tradicional Chinesa , Fígado/metabolismo , Bactérias , Chá
15.
Proc Natl Acad Sci U S A ; 120(12): e2219950120, 2023 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-36913567

RESUMO

High areal capacitance for a practical supercapacitor electrode requires both large mass loading and high utilization efficiency of electroactive materials, which presents a great challenge. Herein, we demonstrated the unprecedented synthesis of superstructured NiMoO4@CoMoO4 core-shell nanofiber arrays (NFAs) on a Mo-transition-layer-modified nickel foam (NF) current collector as a new material, achieving the synergistic combination of highly conductive CoMoO4 and electrochemical active NiMoO4. Moreover, this superstructured material exhibited a large gravimetric capacitance of 1,282.2 F/g in 2 M KOH with a mass loading of 7.8 mg/cm2, leading to an ultrahigh areal capacitance of 10.0 F/cm2 that is larger than any reported values of CoMoO4 and NiMoO4 electrodes. This work provides a strategic insight for rational design of electrodes with high areal capacitances for supercapacitors.

16.
J Environ Manage ; 332: 117398, 2023 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-36738721

RESUMO

Capturing CO2 has become increasingly important. However, wide industrial applications of conventional CO2 capture technologies are limited by their slow CO2 sorption and desorption kinetics. Accordingly, this research is designed to overcome the challenge by synthesizing mesoporous MgO nanoparticles (MgO-NPs) with a new method that uses PEG 1500 as a soft template. MgO surface structure is nonstoichiometric due to its distinctive shape; the abundant Lewis base sites provided by oxygen vacancies promote CO2 capture. Adding 2 wt % MgO-NPs to 20 wt % monoethanolamine (MEA) can increase the breakthrough time (the time with 90% CO2 capturing efficiency) by ∼3000% and can increase the CO2 absorption capacity within the breakthrough time by ∼3660%. The data suggest that MgO-NPs can accelerate the rate and increase CO2 desorption capacity by up to ∼8740% and ∼2290% at 90 °C, respectively. Also, the excellent stability of the system within 50 cycles is verified. These findings demonstrate a new strategy to innovate MEA absorbents currently widely used in commercial post-combustion CO2 capture plants.


Assuntos
Dióxido de Carbono , Óxido de Magnésio , Dióxido de Carbono/química , Óxido de Magnésio/química , Bases de Lewis , Etanolamina/química , Cinética
17.
Chemosphere ; 322: 138174, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36806807

RESUMO

Converting waste plastic into valuable carbon materials as the electrode for supercapacitors represents a sustainable way to deal with the severe waste plastic-related environmental issues. However, ideal carbon materials for supercapacitors require not only a large specific surface area but also abundant meso/macropores, which is still challenging for conventional synthesis methods. Herein, MgO-templated pyrolysis with chemical activation was demonstrated as an effective approach to convert waste polyethylene terephthalate (PET) plastic bottles into 3D meso/macroporous carbon (MMPC) with both large total surface area (1863.55 m2/g) and meso/macropore surface area (1478.46 m2/g). Furthermore, it exhibited a high capacitance of 191.4 F/g and an excellent rate capability (86.3% retention from 0.5 to 10 A/g) for supercapacitor. This work provides not only a facile approach to synthesize 3D meso/macroporous carbon materials but also a sustainable way to mitigate plastic-derived pollution.


Assuntos
Carbono , Plásticos , Óxido de Magnésio , Pirólise , Porosidade , Eletrodos
20.
J Phys Chem Lett ; 14(1): 1-8, 2023 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-36562535

RESUMO

Sodium hydride (NaH) was unprecedently embedded inside graphene nanobubbles via the discovered reaction between NaH and CO. With the graphene nanobubble as a nanoreactor for NaH, we directly observed the electron-beam-induced decomposition process of graphene-covered NaH by in situ high-resolution transmission electron microscopy with energy dispersive spectrometry and electron energy loss spectroscopy, revealing its decomposition mechanism. This can provide guidance for the design of hydrogen storage materials.

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