| 1. |
- Sampson, Joshua N., et al.
(författare)
-
Analysis of Heritability and Shared Heritability Based on Genome-Wide Association Studies for 13 Cancer Types
- 2015
-
Ingår i: Journal of the National Cancer Institute. - : Oxford University Press (OUP). - 0027-8874 .- 1460-2105. ; 107:12
-
Tidskriftsartikel (refereegranskat)abstract
- Background: Studies of related individuals have consistently demonstrated notable familial aggregation of cancer. We aim to estimate the heritability and genetic correlation attributable to the additive effects of common single-nucleotide polymorphisms (SNPs) for cancer at 13 anatomical sites. Methods: Between 2007 and 2014, the US National Cancer Institute has generated data from genome-wide association studies (GWAS) for 49 492 cancer case patients and 34 131 control patients. We apply novel mixed model methodology (GCTA) to this GWAS data to estimate the heritability of individual cancers, as well as the proportion of heritability attributable to cigarette smoking in smoking-related cancers, and the genetic correlation between pairs of cancers. Results: GWAS heritability was statistically significant at nearly all sites, with the estimates of array-based heritability, h(l)(2), on the liability threshold (LT) scale ranging from 0.05 to 0.38. Estimating the combined heritability of multiple smoking characteristics, we calculate that at least 24% (95% confidence interval [CI] = 14% to 37%) and 7% (95% CI = 4% to 11%) of the heritability for lung and bladder cancer, respectively, can be attributed to genetic determinants of smoking. Most pairs of cancers studied did not show evidence of strong genetic correlation. We found only four pairs of cancers with marginally statistically significant correlations, specifically kidney and testes (rho = 0.73, SE = 0.28), diffuse large B-cell lymphoma (DLBCL) and pediatric osteosarcoma (rho = 0.53, SE = 0.21), DLBCL and chronic lymphocytic leukemia (CLL) (rho = 0.51, SE = 0.18), and bladder and lung (rho = 0.35, SE = 0.14). Correlation analysis also indicates that the genetic architecture of lung cancer differs between a smoking population of European ancestry and a nonsmoking Asian population, allowing for the possibility that the genetic etiology for the same disease can vary by population and environmental exposures. Conclusion: Our results provide important insights into the genetic architecture of cancers and suggest new avenues for investigation.
|
|
| 2. |
- Li, Gang, et al.
(författare)
-
Selective Electrochemical Alkaline Seawater Oxidation Catalyzed by Cobalt Carbonate Hydroxide Nanorod Arrays with Sequential Proton-Electron Transfer Properties
- 2021
-
Ingår i: ACS Sustainable Chemistry and Engineering. - : American Chemical Society (ACS). - 2168-0485. ; 9:2, s. 905-913
-
Tidskriftsartikel (refereegranskat)abstract
- Seawater oxygen evolution is one of the promising energy conversion technologies for large-scale renewable energy storage. It requires efficient catalysts to accelerate the oxygen evolution reaction (OER) for sustained water oxidation, avoiding chlorine evolution under acidic conditions or hypochlorite formation in alkaline solutions. Conventional metal oxide-based OER catalysts follow the adsorbate evolution mechanism that involves concerted proton-electron transfer steps at the active sites. Thus, on the scale of reversible hydrogen electrode, their catalytic activity is independent of the pH of electrolytes. In the present study, nanostructured cobalt carbonate hydroxide (CoCH) with sequential proton-electron transfer properties was tested as a catalyst for seawater oxygen evolution. CoCH exhibited pH-dependent water oxidation activities, thereby providing larger potential and current operating windows for selective water oxidation compared to the catalysts with pH-independent OER activities. The operating window can be further expanded by increasing the pH of the electrolyte.
|
|
| 3. |
- Li, Yingzheng, et al.
(författare)
-
Influence of O-O formation pathways and charge transfer mediator on lipid bilayer membrane-like photoanodes for water oxidation
- 2024
-
Ingår i: Journal of Energy Chemistry. - : Elsevier. - 2095-4956 .- 2096-885X. ; 93, s. 526-537
-
Tidskriftsartikel (refereegranskat)abstract
- Inspired by the function of crucial components in photosystem II (PSII), electrochemical and dyesensitized photoelectrochemical (DSPEC) water oxidation devices were constructed by the selfassembly of well-designed amphipathic Ru(bda)-based catalysts (bda = 2,2'-bipyrdine-6,6'-dicarbonoxyl acid) and aliphatic chain decorated electrode surfaces, forming lipid bilayer membrane (LBM)-like structures. The Ru(bda) catalysts on electrode-supported LBM films demonstrated remarkable water oxidation performance with different O-O formation mechanisms. However, compared to the slow charge transfer process, the O-O formation pathways did not determine the PEC water oxidation efficiency of the dyesensitized photoanodes, and the different reaction rates for similar catalysts with different catalytic paths did not determine the PEC performance of the DSPECs. Instead, charge transfer plays a decisive role in the PEC water oxidation rate. When an indolo[3,2-b] carbazole derivative was introduced between the Ru (bda) catalysts and aliphatic chain-modified photosensitizer in LBM films, serving as a charge transfer mediator for the tyrosine-histidine pair in PSII, the PEC water oxidation performance of the corresponding photoanodes was dramatically enhanced.
|
|
| 4. |
- Liu, Chang, et al.
(författare)
-
A dendritic Sb2Se3/In2S3 heterojunction nanorod array photocathode decorated with a MoSx catalyst for efficient solar hydrogen evolution
- 2020
-
Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7488 .- 2050-7496. ; 8:44, s. 23385-23394
-
Tidskriftsartikel (refereegranskat)abstract
- Developing cost-effective photocathodes that show desirable performance for use in commercial photoelectrochemical water splitting devices remains a fundamental and practical challenge. Sb2Se3 semiconductors satisfy most of the demands expected for an ideal highly efficient photocathode, including favorable cost and optoelectronic properties. Herein, we have demonstrated outstanding photoelectrodes using a noble-metal-free catalyst, namely, a MoSx-decorated low-cost Sb2Se3/In2S3 heterojunction, as the photocathode. This enabled a maximum photocurrent density of up to -27 mA cm(-2) (0 V vs. RHE, 100 mW cm(-2), AM 1.5G filter) with a remarkable half solar-to-hydrogen conversion efficiency (STH) of 2.6%, obtained via decreasing charge recombination and accelerating charge transfer through morphological optimization of the In2S3 layer.
|
|
| 5. |
- Zhao, Yilong, et al.
(författare)
-
Efficient urea electrosynthesis from carbon dioxide and nitrate via alternating Cu–W bimetallic C–N coupling sites
- 2023
-
Ingår i: Nature Communications. - : Springer Nature. - 2041-1723. ; 14:1
-
Tidskriftsartikel (refereegranskat)abstract
- Electrocatalytic urea synthesis is an emerging alternative technology to the traditional energy-intensive industrial urea synthesis protocol. Novel strategies are urgently needed to promote the electrocatalytic C–N coupling process and inhibit the side reactions. Here, we report a CuWO4 catalyst with native bimetallic sites that achieves a high urea production rate (98.5 ± 3.2 μg h−1 mg−1cat) for the co-reduction of CO2 and NO3− with a high Faradaic efficiency (70.1 ± 2.4%) at −0.2 V versus the reversible hydrogen electrode. Mechanistic studies demonstrated that the combination of stable intermediates of *NO2 and *CO increases the probability of C–N coupling and reduces the potential barrier, resulting in high Faradaic efficiency and low overpotential. This study provides a new perspective on achieving efficient urea electrosynthesis by stabilizing the key reaction intermediates, which may guide the design of other electrochemical systems for high-value C–N bond-containing chemicals.
|
|
| 6. |
- Li, Yingzheng, et al.
(författare)
-
Switching the O-O Bond Formation Pathways of Ru-pda Water Oxidation Catalyst by Third Coordination Sphere Engineering
- 2021
-
Ingår i: RESEARCH. - : American Association for the Advancement of Science (AAAS). - 2639-5274. ; 2021
-
Tidskriftsartikel (refereegranskat)abstract
- Water oxidation is a vital anodic reaction for renewable fuel generation via electrochemical- and photoelectrochemical-driven water splitting or CO2 reduction. Ruthenium complexes, such as Ru-bda family, have been shown as highly efficient water-oxidation catalysts (WOCs), particularly when they undergo a bimolecular O-O bond formation pathway. In this study, a novel Ru(pda)-type (pda(2-) = 1,10-phenanthroline-2,9-dicarboxylate) molecular WOC with 4-vinylpyridine axial ligands was immobilized on the glassy carbon electrode surface by electrochemical polymerization. Electrochemical kinetic studies revealed that this homocoupling polymer catalyzes water oxidation through a bimolecular radical coupling pathway, where interaction between two Ru(pda)-oxyl moieties (I2M) forms the O-O bond. The calculated barrier of the I2M pathway by density-functional theory (DFT) is significantly lower than the barrier of a water nucleophilic attack (WNA) pathway. By using this polymerization strategy, the Ru centers are brought closer in the distance, and the O-O bond formation pathway by the Ru (pda) catalyst is switched from WNA in a homogeneous molecular catalytic system to I2M in the polymerized film, providing some deep insights into the importance of third coordination sphere engineering of the water oxidation catalyst.
|
|
| 7. |
- Dong, Zhihua, et al.
(författare)
-
Thermo-mechanical properties of Cr-Co-Ni alloys from longitudinal spin fluctuation theory
- 2021
-
Ingår i: Applied Physics Letters. - : AIP Publishing. - 0003-6951 .- 1077-3118. ; 119:8
-
Tidskriftsartikel (refereegranskat)abstract
- Accounting for longitudinal spin fluctuations in the paramagnetic state, we calculate elastic constants and stacking fault energy as a function of temperature and chemical composition for Cr-Co-Ni alloys. The longitudinal spin fluctuations are demonstrated to be important for the quantitative description of the thermo-mechanical properties and the corresponding chemical and temperature dependences. Replacing Ni with Cr and Co is found to yield opposite influence on the mechanical properties at finite temperature. A high thermal stability in plasticity is predicted in the low Cr regime in Cr-Co-Ni alloys, while a good thermal stability in elasticity can be achieved in the high Cr and low Co regime. The present advance in thermo-chemical-magnetic-property enhances the understanding required for an intelligent design of multicomponent alloys toward high-technology applications. Published under an exclusive license by AIP Publishing.
|
|
| 8. |
- Duan, Lele, et al.
(författare)
-
Highly Efficient Bioinspired Molecular Ru Water Oxidation Catalysts with Negatively Charged Backbone Ligands
- 2015
-
Ingår i: Accounts of Chemical Research. - : American Chemical Society (ACS). - 0001-4842 .- 1520-4898. ; 48:7, s. 2084-2096
-
Forskningsöversikt (refereegranskat)abstract
- The oxygen evolving complex (OEC) of the natural photosynthesis system II (PSII) oxidizes water to produce oxygen and reducing equivalents (protons and electrons). The oxygen released from PSII provides the oxygen source of our atmosphere; the reducing equivalents are used to reduce carbon dioxide to organic products, which support almost all organisms on the Earth planet. The first photosynthetic organisms able to split water were proposed to be cyanobacteria-like ones appearing ca. 2.5 billion years ago. Since then, nature has chosen a sustainable way by using solar energy to develop itself. Inspired by nature, human beings started to mimic the functions of the natural photosynthesis system and proposed the concept of artificial photosynthesis (AP) with the view to creating energy-sustainable societies and reducing the impact on the Earth environments. Water oxidation is a highly energy demanding reaction and essential to produce reducing equivalents for fuel production, and thereby effective water oxidation catalysts (WOCs) are required to catalyze water oxidation and reduce the energy loss. X-ray crystallographic studies on PSII have revealed that the OEC consists of a Mn4CaO5 cluster surrounded by oxygen rich ligands, such as oxyl, oxo, and carboxylate ligands. These negatively charged, oxygen rich ligands strongly stabilize the high valent states of the Mn cluster and play vital roles in effective water oxidation catalysis with low overpotential. This Account describes our endeavors to design effective Ru WOCs with low overpotential, large turnover number, and high turnover frequency by introducing negatively charged ligands, such as carboxylate. Negatively charged ligands stabilized the high valent states of Ru catalysts, as evidenced by the low oxidation potentials. Meanwhile, the oxygen production rates of our Ru catalysts were improved dramatically as well. Thanks to the strong electron donation ability of carboxylate containing ligands, a seven-coordinate Ru-IV species was isolated as a reaction intermediate, shedding light on the reaction mechanisms of Ru-catalyzed water oxidation chemistry. Auxiliary ligands have dramatic effects on the water oxidation catalysis in terms of the reactivity and the reaction mechanism. For instance, Ru-bda (H(2)bda = 2,2'-bipyridine-6,6'-dicarboxylic acid) water oxidation catalysts catalyze Ce-IV-driven water oxidation extremely fast via the radical coupling of two Ru-V=O species, while Ru-pda (H(2)pda = 1,10-phenanthroline-2,9-dicarboxylic acid) water oxidation catalysts catalyze the same reaction slowly via water nucleophilic attack on a Ru-V-O species. With a number of active Ru catalysts in hands, light driven water oxidation was accomplished using catalysts with low catalytic onset potentials. The structures of molecular catalysts could be readily tailored to introduce additional functional groups, which favors the fabrication of state-of-the-art Ru-based water oxidation devices, such as electrochemical water oxidation anodes and photo-electrochemical anodes. The development of efficient water oxidation catalysts has led to a step forward in the sustainable energy system.
|
|
| 9. |
- Li, Fusheng, et al.
(författare)
-
Device Fabrication for Water Oxidation, Hydrogen Generation, and CO2 Reduction via Molecular Engineering
- 2018
-
Ingår i: Joule. - : CELL PRESS. - 2542-4351. ; 2:1, s. 36-60
-
Tidskriftsartikel (refereegranskat)abstract
- Research on the storage of solar energy in terms of hydrogen or carbon-based fuels by using sunlight to split water or to reduce CO2, respectively, has gained significant attention in recent years. Among reported water-splitting systems, one approach has focused on hybrid systems with molecular catalysts or molecular light-harvesting systems that are combined with nanostructured materials. In this perspective we summarize recent developments in operation and fabrication strategies for various water-splitting devices constructed from electrodes (electrochemical cells) or photoelectrodes (photoelectrochemical cells) using molecular engineering. We also provide insights into the factors that influence device efficiency and stability, and provide guidelines for future fabrication strategies for more advanced devices.
|
|
| 10. |
- Li, Fusheng, 1985-, et al.
(författare)
-
Electroless Plating of NiFeP Alloy on the Surface of Silicon Photoanode for Efficient Photoelectrochemical Water Oxidation
- 2020
-
Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 12:10, s. 11479-11488
-
Tidskriftsartikel (refereegranskat)abstract
- N- type silicon is a kind of semiconductor with a narrow band gap that has been reported as an outstanding light-harvesting material for photoelectrochemical (PEC) reactions. Decorating a thin catalyst layer on the n-type silicon surface can provide a direct and effective route toward PEC water oxidation. However, most of catalyst immobilization methods for reported n-type silicon photoanodes have been based on energetically demanding, time-consuming, and high-cost processes. Herein, a high-performance NiFeP alloy (NiFeP)-decorated n-type micro-pyramid silicon array (n-Si) photoanode (NiFeP/n-Si) was prepared by a fast and low-cost electroless deposition method for light-driven water oxidation reaction. The saturated photocurrent density of NiFeP/n-Si can reach up to similar to 40 mA cm(-2) and a photocurrent density of 15.5 mA cm(-2) can be achieved at 1.23 V-RHE under light illumination (100 mW cm(-2), AM1.5 filter), which is one of the most promising silicon-based photoanodes to date. The kinetic studies showed that the NiFeP on the silicon photoanodes could significantly decrease the interfacial charge recombination between the n-type silicon surface and electrolyte.
|
|
