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913 result(s) for "Wang, Hailiang"
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Domino electroreduction of CO2 to methanol on a molecular catalyst
Electrochemical carbon dioxide (CO 2 ) reduction can in principle convert carbon emissions to fuels and value-added chemicals, such as hydrocarbons and alcohols, using renewable energy, but the efficiency of the process is limited by its sluggish kinetics 1 , 2 . Molecular catalysts have well defined active sites and accurately tailorable structures that allow mechanism-based performance optimization, and transition-metal complexes have been extensively explored in this regard. However, these catalysts generally lack the ability to promote CO 2 reduction beyond the two-electron process to generate more valuable products 1 , 3 . Here we show that when immobilized on carbon nanotubes, cobalt phthalocyanine—used previously to reduce CO 2 to primarily CO—catalyses the six-electron reduction of CO 2 to methanol with appreciable activity and selectivity. We find that the conversion, which proceeds via a distinct domino process with CO as an intermediate, generates methanol with a Faradaic efficiency higher than 40 per cent and a partial current density greater than 10 milliamperes per square centimetre at −0.94 volts with respect to the reversible hydrogen electrode in a near-neutral electrolyte. The catalytic activity decreases over time owing to the detrimental reduction of the phthalocyanine ligand, which can be suppressed by appending electron-donating amino substituents to the phthalocyanine ring. The improved molecule-based electrocatalyst converts CO 2 to methanol with considerable activity and selectivity and with stable performance over at least 12 hours. Individual cobalt phthalocyanine derivative molecules immobilized on carbon nanotubes effectively catalyse the electroreduction of CO 2 to methanol via a domino process with high activity and selectivity and stable performance.
High-capacity rechargeable batteries based on deeply cyclable lithium metal anodes
Discovering new chemistry and materials to enable rechargeable batteries with higher capacity and energy density is of paramount importance. While Li metal is the ultimate choice of a battery anode, its low efficiency is still yet to be overcome. Many strategies have been developed to improve the reversibility and cycle life of Li metal electrodes. However, almost all of the results are limited to shallow cycling conditions (e.g., 1 mAh cm−2) and thus inefficient utilization (<1%). Here we achieve Li metal electrodes that can be deeply cycled at high capacities of 10 and 20 mAh cm−2 with average Coulombic efficiency >98% in a commercial LiPF₆/carbonate electrolyte. The high performance is enabled by slow release of LiNO₃ into the electrolyte and its subsequent decomposition to form a Li₃N and lithium oxynitrides (LiNₓOy)-containing protective layer which renders reversible, dendrite-free, and highly dense Li metal deposition. Using the developed Li metal electrodes, we construct a Li-MoS₃ full cell with the anode and cathode materials in a close-to-stoichiometric amount ratio. In terms of both capacity and energy, normalized to either the electrode area or the total mass of the electrode materials, our cell significantly outperforms other laboratory-scale battery cells as well as the state-of-the-art Li ion batteries on the market.
Co3O4 nanocrystals on graphene as a synergistic catalyst for oxygen reduction reaction
Catalysts for oxygen reduction and evolution reactions are at the heart of key renewable-energy technologies including fuel cells and water splitting. Despite tremendous efforts, developing oxygen electrode catalysts with high activity at low cost remains a great challenge. Here, we report a hybrid material consisting of Co 3 O 4 nanocrystals grown on reduced graphene oxide as a high-performance bi-functional catalyst for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Although Co 3 O 4 or graphene oxide alone has little catalytic activity, their hybrid exhibits an unexpected, surprisingly high ORR activity that is further enhanced by nitrogen doping of graphene. The Co 3 O 4 /N-doped graphene hybrid exhibits similar catalytic activity but superior stability to Pt in alkaline solutions. The same hybrid is also highly active for OER, making it a high-performance non-precious metal-based bi-catalyst for both ORR and OER. The unusual catalytic activity arises from synergetic chemical coupling effects between Co 3 O 4 and graphene. Developing oxygen-electrode catalysts with high activity at low cost for renewable energy applications such as water splitting and fuel cells is challenging. A hybrid material of Co 3 O 4 nanocrystals grown on reduced graphene oxide exhibits enhanced catalytic performance for the oxygen reduction and oxygen evolution reactions.
Facile synthesis of high-quality graphene nanoribbons
Graphene nanoribbons have attracted attention because of their novel electronic and spin transport properties 1 , 2 , 3 , 4 , 5 , 6 , and also because nanoribbons less than 10 nm wide have a bandgap that can be used to make field-effect transistors 1 , 2 , 3 . However, producing nanoribbons of very high quality, or in high volumes, remains a challenge 1 , 4 , 5 , 6 , 7 , 8 , 9 , 10 , 11 , 12 , 13 , 14 , 15 , 16 , 17 , 18 . Here, we show that pristine few-layer nanoribbons can be produced by unzipping mildly gas-phase oxidized multiwalled carbon nanotubes using mechanical sonication in an organic solvent. The nanoribbons are of very high quality, with smooth edges (as seen by high-resolution transmission electron microscopy), low ratios of disorder to graphitic Raman bands, and the highest electrical conductance and mobility reported so far (up to 5 e 2 / h and 1,500 cm 2  V −1  s −1 for ribbons 10–20 nm in width). Furthermore, at low temperatures, the nanoribbons show phase-coherent transport and Fabry–Perot interference, suggesting minimal defects and edge roughness. The yield of nanoribbons is ∼2% of the starting raw nanotube soot material, significantly higher than previous methods capable of producing high-quality narrow nanoribbons 1 . The relatively high-yield synthesis of pristine graphene nanoribbons will make these materials easily accessible for a wide range of fundamental and practical applications. Unzipping carbon nanotubes that have been mildly gas-phase oxidized results in graphene nanoribbons of very high quality.
Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction
Restructuring-induced catalytic activity is an intriguing phenomenon of fundamental importance to rational design of high-performance catalyst materials. We study three copper-complex materials for electrocatalytic carbon dioxide reduction. Among them, the copper(II) phthalocyanine exhibits by far the highest activity for yielding methane with a Faradaic efficiency of 66% and a partial current density of 13 mA cm −2 at the potential of – 1.06 V versus the reversible hydrogen electrode. Utilizing in-situ and operando X-ray absorption spectroscopy, we find that under the working conditions copper(II) phthalocyanine undergoes reversible structural and oxidation state changes to form ~ 2 nm metallic copper clusters, which catalyzes the carbon dioxide-to-methane conversion. Density functional calculations rationalize the restructuring behavior and attribute the reversibility to the strong divalent metal ion–ligand coordination in the copper(II) phthalocyanine molecular structure and the small size of the generated copper clusters under the reaction conditions. The catalytic conversion of carbon dioxide into value-added products requires an understanding of the active species present under working conditions. Here, the authors discover copper-containing complexes to reversibly transform during electrocatalysis into methane-producing copper nanoclusters.
RNA-Seq analysis of salinity stress–responsive transcriptome in the liver of spotted sea bass (Lateolabrax maculatus)
Salinity is one of the most prominent abiotic factors, which greatly influence reproduction, development, growth, physiological and metabolic activities of fishes. Spotted sea bass (Lateolabrax maculatus), as a euryhaline marine teleost, has extraordinary ability to deal with a wide range of salinity changes. However, this species is devoid of genomic resources, and no study has been conducted at the transcriptomic level to determine genes responsible for salinity regulation, which impedes the understanding of the fundamental mechanism conferring tolerance to salinity fluctuations. Liver, as the major metabolic organ, is the key source supplying energy for iono- and osmoregulation in fish, however, little attention has been paid to its salinity-related functions but which should not be ignored. In this study, we perform RNA-Seq analysis to identify genes involved in salinity adaptation and osmoregulation in liver of spotted sea bass, generating from the fishes exposed to low and high salinity water (5 vs 30ppt). After de novo assembly, annotation and differential gene expression analysis, a total of 455 genes were differentially expressed, including 184 up-regulated and 271 down-regulated transcripts in low salinity-acclimated fish group compared with that in high salinity-acclimated group. A number of genes with a potential role in salinity adaptation for spotted sea bass were classified into five functional categories based on the gene ontology (GO) and enrichment analysis, which include genes involved in metabolites and ion transporters, energy metabolism, signal transduction, immune response and structure reorganization. The candidate genes identified in L. maculates liver provide valuable information to explore new pathways related to fish salinity and osmotic regulation. Besides, the transcriptomic sequencing data supplies significant resources for identification of novel genes and further studying biological questions in spotted sea bass.
Highly selective and active CO2 reduction electrocatalysts based on cobalt phthalocyanine/carbon nanotube hybrid structures
Electrochemical reduction of carbon dioxide with renewable energy is a sustainable way of producing carbon-neutral fuels. However, developing active, selective and stable electrocatalysts is challenging and entails material structure design and tailoring across a range of length scales. Here we report a cobalt-phthalocyanine-based high-performance carbon dioxide reduction electrocatalyst material developed with a combined nanoscale and molecular approach. On the nanoscale, cobalt phthalocyanine (CoPc) molecules are uniformly anchored on carbon nanotubes to afford substantially increased current density, improved selectivity for carbon monoxide, and enhanced durability. On the molecular level, the catalytic performance is further enhanced by introducing cyano groups to the CoPc molecule. The resulting hybrid catalyst exhibits >95% Faradaic efficiency for carbon monoxide production in a wide potential range and extraordinary catalytic activity with a current density of 15.0 mA cm −2 and a turnover frequency of 4.1 s −1 at the overpotential of 0.52 V in a near-neutral aqueous solution. Electrochemical reduction of carbon dioxide is a sustainable way of producing carbon-neutral fuels. Here, the authors take a combined nanoscale and molecular approach to develop a highly active and selective cobalt phthalocyanine/carbon nanotube hybrid electrocatalyst for carbon dioxide reduction to carbon monoxide.
Advanced zinc-air batteries based on high-performance hybrid electrocatalysts
Primary and rechargeable Zn-air batteries could be ideal energy storage devices with high energy and power density, high safety and economic viability. Active and durable electrocatalysts on the cathode side are required to catalyse oxygen reduction reaction during discharge and oxygen evolution reaction during charge for rechargeable batteries. Here we developed advanced primary and rechargeable Zn-air batteries with novel CoO/carbon nanotube hybrid oxygen reduction catalyst and Ni-Fe-layered double hydroxide oxygen evolution catalyst for the cathode. These catalysts exhibited higher catalytic activity and durability in concentrated alkaline electrolytes than precious metal Pt and Ir catalysts. The resulting primary Zn-air battery showed high discharge peak power density ~265 mW cm −2 , current density ~200 mA cm −2 at 1 V and energy density >700 Wh kg −1 . Rechargeable Zn-air batteries in a tri-electrode configuration exhibited an unprecedented small charge–discharge voltage polarization of ~0.70 V at 20 mA cm −2 , high reversibility and stability over long charge and discharge cycles. Metal-air batteries are promising for energy storage because of their high theoretical energy density, but their realization is hampered by the lack of efficient and robust air catalysts. Li et al . construct stable zinc-air batteries using novel catalysts for oxygen reduction and evolution reactions.
An examination of the socio-demographic correlates of patient adherence to self-management behaviors and the mediating roles of health attitudes and self-efficacy among patients with coexisting type 2 diabetes and hypertension
Background Patients with coexisting type 2 diabetes and hypertension generally exhibit poor adherence to self-management, which adversely affects their disease control. Therefore, identification of the factors related to patient adherence is warranted. In this study, we aimed to examine (i) the socio-demographic correlates of patient adherence to a set of self-management behaviors relevant to type 2 diabetes and hypertension, namely, medication therapy, diet therapy, exercise, tobacco and alcohol avoidance, stress reduction, and self-monitoring/self-care, and (ii) whether health attitudes and self-efficacy in performing self-management mediated the associations between socio-demographic characteristics and adherence. Methods We performed a secondary analysis of data collected in a randomized controlled trial. The sample comprised 148 patients with coexisting type 2 diabetes mellitus and hypertension. Data were collected by a questionnaire and analyzed using logistic regression. Results Female patients were found to be less likely to exercise regularly (odds ratio [OR] = 0.49, P  = 0.03) and more likely to avoid tobacco and alcohol (OR = 9.87, P  < 0.001) than male patients. Older patients were found to be more likely to adhere to diet therapy (OR = 2.21, P  = 0.01) and self-monitoring/self-care (OR = 2.17, P  = 0.02). Patients living with family or others (e.g., caregivers) were found to be more likely to exercise regularly (OR = 3.44, P  = 0.02) and less likely to avoid tobacco and alcohol (OR = 0.10, P  = 0.04) than those living alone. Patients with better perceived health status were found to be more likely to adhere to medication therapy (OR = 2.02, P  = 0.03). Patients with longer diabetes duration (OR = 2.33, P  = 0.01) were found to be more likely to adhere to self-monitoring/self-care. Self-efficacy was found to mediate the association between older age and better adherence to diet therapy, while no significant mediating effects were found for health attitudes. Conclusions Adherence to self-management was found to be associated with socio-demographic characteristics (sex, age, living status, perceived health status, and diabetes duration). Self-efficacy was an important mediator in some of these associations, suggesting that patient adherence may be improved by increasing patients’ self-management efficacy, such as by patient empowerment, collaborative care, or enhanced patient–physician interactions.
Phosphorus oxoanion-intercalated layered double hydroxides for high-performance oxygen evolution
Rational design and controlled fabrication of efficient and cost-effective electrodes for the oxygen evolution reaction (OER) are critical for addressing the unpre- cedented energy crisis. Nickel-iron layered double hydroxides (NiFe-LDHs) with specific interlayer anions (i.e. phosphate, phosphite, and hypophosphite) were fabricated by a co-predpitation method and investigated as oxygen evolution electrocatalysts. Intercalation of the phosphorus oxoanion enhanced the OER activity in an alkaline solution; the optimal performance (i.e., a low onset potential of 215 mV, a small Tafel slope of 37.7 mV/dec, and stable electrochemical behavior) was achieved with the hypophosphite-intercalated NiFe-LDH catalyst, demonstrating dramatic enhancement over the traditional carbonate-intercalated NiFe-LDH in terms of activity and durability. This enhanced performance is attributed to the interaction between the intercalated phosphorous oxoanions and the edge-sharing MO6 (M = Ni, Fe) layers, which modifies the surface electronic structure of the Ni sites. This concept should be inspiring for the design of more effective LDH-based oxygen evolution electrocatalvsts.