Hydrogen evolution reaction (HER) from water electrolysis is an ideal alternative solution to address the energy crisis and develop clean energy. However, the construction of an efficient electrocatalyst with multiple...Hydrogen evolution reaction (HER) from water electrolysis is an ideal alternative solution to address the energy crisis and develop clean energy. However, the construction of an efficient electrocatalyst with multiple active sites that can ensure high metal utilization and promote reaction kinetics simultaneously still leaves a major challenge. Herein, we present a facile strategy to synthesize a HER catalyst comprising Pt single atoms (PtSA) anchored in Fe vacancies and Pt quantum dots (Pt_(QD)) on the surface of NiFe LDH. Benefitting from the hierarchical and ultrathin nanosheet arrays and strong electronic interaction between PtSA/Pt_(QD) and NiFe LDH matrix, the optimized sample (Pt_(SA/QD)-NiFe_(V9) LDH) exhibits outstanding HER performance in 1 M KOH with ultra-low overpotentials of 20 and 67 mV at 10 and 100 mA cm^(−2), respectively, outperforming the benchmark Pt/C electrocatalyst. In addition, the electrolyzer using Pt_(SA/QD)-NiFe_(V9) LDH as a cathode requires voltages of only 1.48 and 1.73 V to yield current densities of 10 and 1000 mA cm^(−2), respectively. The combination of in situ tests and density functional theory (DFT) calculations reveal that the synergy of PtSA and Pt_(QD) can optimize the kinetics of water dissociation and hydrogen desorption, thus the Volmer-Tafel pathway prevailing the HER process. This work provides a promising surface engineering strategy to develop catalysts for efficient and robust hydrogen evolution.展开更多
Aluminum(Al)exhibits excellent electrical conductivity,mechanical ductility,and good chemical compatibility with high-ionic-conductivity electrolytes.This makes it more suitable as an anode material for all-solid-stat...Aluminum(Al)exhibits excellent electrical conductivity,mechanical ductility,and good chemical compatibility with high-ionic-conductivity electrolytes.This makes it more suitable as an anode material for all-solid-state lithium batteries(ASSLBs)compared to the overly reactive metallic lithium anode and the mechanically weak silicon anode.This study finds that the pre-lithiated Al anode demonstrates outstanding interfacial stability with the Li_6PS_5Cl(LPSCl)electrolyte,maintaining stable cycling for over 1200 h under conditions of deep charge-discharge.This paper combines the pre-lithiated Al anode with a high-nickel cathode,LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2),paired with the highly ionic conductive LPSCl electrolyte,to design an ASSLB with high energy density and stability.Using anode pre-lithiation techniques,along with dual-reinforcement technology between the electrolyte and the cathode active material,the ASSLB achieves stable cycling for 1000 cycles at a 0.2C rate,with a capacity retention rate of up to 82.2%.At a critical negative-to-positive ratio of 1.1,the battery's specific energy reaches up to 375 Wh kg^(-1),and it maintains over 85.9%of its capacity after 100 charge-discharge cycles.This work provides a new approach and an excellent solution for developing low-cost,high-stability all-solid-state batteries.展开更多
Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance i...Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.展开更多
Large-scale green hydrogen production technology,based on the electrolysis of water powered by renewable energy,relies heavily on non-precious metal oxygen evolution reactions(OER)electrocatalysts with high activity a...Large-scale green hydrogen production technology,based on the electrolysis of water powered by renewable energy,relies heavily on non-precious metal oxygen evolution reactions(OER)electrocatalysts with high activity and stability under industrial conditions(6 M KOH,60℃-80℃)at large current density.Here,we construct Fe and Co co-incorporated nickel(oxy)hydroxide(Fe_(2.5)Co_(2.5)Ni_(10)O_(y)H_(z)@NFF)via a multi-metal electrodeposition,which exhibits outstanding OER performance(overpotential:185 mV@10 mA cm^(-2)).Importantly,an overwhelming stability for more than 1100 h at 500 mA cm^(-2)under industrial conditions is achieved.Our combined experimental and computational investigation reveals the surface-reconstructedγ-NiOOH with a high valence state is the active layer,where the optimal(Fe,Co)co-incorporation tunes its electronic structure,changes the potential determining step,and reduces the energy barrier,leading to ultrahigh activity and stability.Our findings demonstrate a facile way to achieve an electrocatalyst with high performance for the industrial production of green hydrogen.展开更多
Two-dimensional materials have been widely used to tune the growth and energy-level alignment of perovskites.However,their incomplete passivation and chaotic usage amounts are not conducive to the preparation of highq...Two-dimensional materials have been widely used to tune the growth and energy-level alignment of perovskites.However,their incomplete passivation and chaotic usage amounts are not conducive to the preparation of highquality perovskite films.Herein,we succeeded in obtaining higher-quality CsPbBr_(3)films by introducing large-area monolayer graphene as a stable physical overlay on top of TiO_(2)substrates.Benefiting from the inert and atomic smooth graphene surface,the CsPbBr_(3)film grown on top by the van der Waal epitaxy has higher crystallinity,improved(100)orientation,and an average domain size of up to 1.22μm.Meanwhile,a strong downward band bending is observed at the graphene/perovskite interface,improving the electron extraction to the electron transport layers(ETL).As a result,perovskite film grown on graphene has lower photoluminescence(PL)intensity,shorter carrier lifetime,and fewer defects.Finally,a photovoltaic device based on epitaxy CsPbBr_(3)film is fabricated,exhibiting power conversion efficiency(PCE)of up to 10.64%and stability over 2000 h in the air.展开更多
We must urgently synthesize highly efficient and stable oxygen-evolution reaction(OER) catalysts for acidic media. Herein, we constructed a series of Ti mesh(TM)-supported RuO_(2)/CoMo_(y)O_(x) catalysts(RuO_(2)/CoMo_...We must urgently synthesize highly efficient and stable oxygen-evolution reaction(OER) catalysts for acidic media. Herein, we constructed a series of Ti mesh(TM)-supported RuO_(2)/CoMo_(y)O_(x) catalysts(RuO_(2)/CoMo_(y)O_(x)/TM) with heterogeneous structures. By optimizing the ratio of Co to Mo, RuO_(2)/CoMO_(2)O_(x)/TM with low Ru loading(0.079 mg/cm^(2)) achieves remarkable OER performance(η = 243 mV at 10 mA/cm^(2)) and high stability(300 h @ 10 mA/cm^(2)) in 0.5 mol/L H_(2)SO_(4) electrolyte. The activity of RuO_(2)/CoMo_yO_x/TM can be maintained for 50 h at 100 mA/cm^(2), and a water electrolyzer with RuO_(2)/CoMO_(2)O_(x)/TM as anode can operate for 40 h at 100 mA/cm~2, suggesting the remarkable OER durability of RuO_(2)/CoMo__(y)O__(x)/TM in acidic electrolyte. Owing to the heterogeneous interface between CoMO_(2)O_(x) and RuO_(2), the electronic structure of Ru atoms was optimized and electron-rich Ru was formed. With modulated electronic properties, the dissociation energy of H_(2)O is weakened, and the OER barrier is lowered. This study provides the design of low-cost noble metal catalysts with long-term stability in an acidic environment.展开更多
The relationship between the protective performance of flexible polymer material and material parameters(elasticmodulus,viscosity coefficient)is explored,an impact collision motion equation between two bodies is estab...The relationship between the protective performance of flexible polymer material and material parameters(elasticmodulus,viscosity coefficient)is explored,an impact collision motion equation between two bodies is establishedfrom the viscoelastic material constitutive,and the relationship between the kinematic response and the materialparameters is obtained.Based on the Kelvin constitutive model,a theoretical model for impact between the pro-tective body and the protected body is established,then the dynamic response is obtained.The feasibility of themodel was verified by drop hammer experiment,and the material parameters(elastic modulus,viscosity coeffi-cient)were obtained by formula.The model is discretized and the relationship between local impact response andmaterial parameters is analyzed.The discussion results on the relationship between the impact response and theprotective material performance indicate that adjusting the elastic modulus,viscosity coefficient,and thicknessof the protective material can effectively improve protective effect.展开更多
<strong>Background: </strong>Studies have shown that long non-coding RNA (LncRNA) plays a critical role in maintaining genomic instability. The correlation between lncRNA and genomic instability is still w...<strong>Background: </strong>Studies have shown that long non-coding RNA (LncRNA) plays a critical role in maintaining genomic instability. The correlation between lncRNA and genomic instability is still worth exploring in bladder cancer as a new tumour marker. <strong>Methods: </strong>Therefore, combined with the lncRNA expression profile and somatic mutation profile of bladder cancer, we established a computing framework of lncRNA related to genomic instability and identified 58 new lncRNA related to genomic instability. Next, we identified a lncRNA signature (GILncSig), based on these 58 new genes, which divided patients into high-risk and low-risk groups. The clinical prognosis was significantly different and was further verified in an independent cohort of patients. <strong>Results: </strong>We confirmed that GILncSig is related to the genomic mutation rate of bladder cancer, suggesting that GILncSig can be used as an indicator of genomic instability. The results show that GILncSig has prognostic value independent of age, sex, grade, and stage and is vital in evaluating clinical prognosis. To sum up, this study provides a vital research basis and methods for further exploring the role of lncRNA in the genomic instability of bladder cancer and provides a theoretical basis for the identification of bladder cancer biomarkers related to genomic instability.展开更多
In maxillofacial surgery, there is a significant need for the design and fabrication of porous scaffolds with customizable bionic structures and mechanical properties suitable for bone tissue engineering. In this pape...In maxillofacial surgery, there is a significant need for the design and fabrication of porous scaffolds with customizable bionic structures and mechanical properties suitable for bone tissue engineering. In this paper, we characterize the porous Ti6Al4V implant, which is one of the most promising and attractive biomedical applications due to the similarity of its modulus to human bones. We describe the mechanical properties of this implant, which we suggest is capable of providing important biological functions for bone tissue regeneration. We characterize a novel bionic design and fabrication process for porous implants. A design concept of “reducing dimensions and designing layer by layer” was used to construct layered slice and rod-connected mesh structure (LSRCMS) implants. Porous LSRCMS implants with different parameters and porosities were fabricated by selective laser melting (SLM). Printed samples were evaluated by microstructure characterization, specific mechanical properties were analyzed by mechanical tests, and finite element analysis was used to digitally calculate the stress characteristics of the LSRCMS under loading forces. Our results show that the samples fabricated by SLM had good structure printing quality with reasonable pore sizes. The porosity, pore size, and strut thickness of manufactured samples ranged from (60.95± 0.27)% to (81.23±0.32)%,(480±28) to (685±31)μm, and (263±28) to (265±28)μm, respectively. The compression results show that the Young’s modulus and the yield strength ranged from (2.23±0.03) to (6.36±0.06) GPa and (21.36±0.42) to (122.85±3.85) MPa, respectively. We also show that the Young’s modulus and yield strength of the LSRCMS samples can be predicted by the Gibson-Ashby model. Further, we prove the structural stability of our novel design by finite element analysis. Our results illustrate that our novel SLM-fabricated porous Ti6Al4V scaffolds based on an LSRCMS are a promising material for bone implants, and are potentially applicable to the field of bone defect repair.展开更多
BACKGROUND Patients with hypothalamic-pituitary disease have the feature of central obesity,insulin resistance, and dyslipidemia, and there is increased prevalence of liver dysfunction consistent with non-alcoholic fa...BACKGROUND Patients with hypothalamic-pituitary disease have the feature of central obesity,insulin resistance, and dyslipidemia, and there is increased prevalence of liver dysfunction consistent with non-alcoholic fatty liver disease(NAFLD) in this population. The causes of hypopituitarism in the reported studies varied and combined pituitary hormone deficiency including central diabetes insipidus is much common in this population. This retrospective cross-sectional study was performed to analyze the clinical characteristics and related factors with NAFLD and cirrhosis in Chinese adult hypopituitary/panhypopituitary patients.AIM To analyze the clinical characteristics of and related risk factors for NAFLD in Chinese adult hypopituitary patients.METHODS Adult Chinese patients with hypopituitarism and/or panhypopituitarism were enrolled at the Pituitary Center of Peking Union Medical College Hospitalbetween August 2012 and April 2018. According to abdominal ultrasonography,these patients were divided into an NAFLD(-) group and an NAFLD(+) group,and the latter was further divided into an NAFLD group and a cirrhotic group.The data, such as patient characteristics, diagnosis, and treatment, were extracted from medical records, and statistical analysis was performed.RESULTS A total of 36 male and 14 female adult Chinese patients with hypopituitarism were included in this retrospective study; 43(87.0%) of these patients exhibited growth hormone(GH) deficiency, and 39(78.3%) had diabetes insipidus. A total of 27(54.0%) patients were diagnosed with NAFLD, while seven patients were cirrhotic. No significant differences were noted in serum GH or insulin-like growth factor 1 among patients with cirrhosis, subjects with NAFLD, and those without NAFLD. However, plasma osmolality and serum sodium concentration of the cirrhotic patients were 314.9 mOsm/kgH2 O and 151.0 mmol/L,respectively, which were significantly higher than those of the NAFLD patients(P = 0.036 and 0.042, respectively). Overweight/obesity and insulin resistance were common metabolic disorders in this population. The body mass index(BMI)and homeostasis model assessment of insulin resistance parameters of the cirrhotic patients were 27.7 kg/m2 and 9.57, respectively, which were significantly higher than those of the patients without NAFLD(P = 0.011 and0.044, respectively). A correlation analysis was performed, and fasting insulin concentration was positively associated with plasma osmolality in patients with NAFLD, after adjusting for gender, age, and BMI(r = 0.540, P = 0.046), but no correlation was noted in patients without NAFLD.CONCLUSION NAFLD is common in patients with hypopituitarism. Plasma osmolality and serum sodium levels of hypopituitary patients with cirrhosis are higher than those of subjects with NAFLD, and fasting insulin concentration is positively associated with plasma osmolality in patients with NAFLD, which suggests that hyperosmolality might be a contributor to the worsening of NAFLD in hypopituitary patients.展开更多
Oxygen evolution reaction(OER)is a critical process in electrocatalytic water splitting.However,the development of low-cost,highly efficient OER electrocatalysts by a simple method that can be used for industrial appl...Oxygen evolution reaction(OER)is a critical process in electrocatalytic water splitting.However,the development of low-cost,highly efficient OER electrocatalysts by a simple method that can be used for industrial application on a large scale is still a huge challenge.Recently,high entropy alloy(HEA)has acquired extensive attention,which may provide answers to the current dilemma.Here,we report bulk Fe_(50)Mn_(30)Co_(10)Cr_(10),which is prepared by 3D printing on a large scale,as electrocatalyst for OER with high catalytic performance.Especially,an easy approach,corrosion engineering,is adopted for the first time to build an active layer of honeycomb nanostructures on its surface,leading to ultrahigh OER performance with an overpotential of 247 mV to achieve a current density of 10 mA cm^(-2),a low Tafel slope of 63 mV dec^(-1),and excellent stability up to 60 h at 100 mA cm^(-2)in 1 M KOH.The excellent catalytic activity mainly originates from:(1)the binder-free self-supported honeycomb nanostructures and multi-component hydroxides,which improve intrinsic catalytic activity,provide rich active sites,and reduce interfacial resistance;and(2)the diverse valence states for multiple active sites to enhance the OER kinetics.Our findings show that corrosion engineering is a novel strategy to improve the bulk HEA catalytic performance.We expect that this work would open up a new avenue to fabricate large-scale HEA electrocatalysts by 3D printing and corrosion engineering for industrial applications.展开更多
The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both hav...The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O_(2) to water(H_2O) or from O_(2) to hydrogen peroxide(H_2O_(2)). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments(e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges.展开更多
Lithium–sulfur(Li–S) batteries have received widespread attention, and lean electrolyte Li–S batteries have attracted additional interest because of their higher energy densities. This review systematically analyze...Lithium–sulfur(Li–S) batteries have received widespread attention, and lean electrolyte Li–S batteries have attracted additional interest because of their higher energy densities. This review systematically analyzes the effect of the electrolyte-to-sulfur(E/S) ratios on battery energy density and the challenges for sulfur reduction reactions(SRR) under lean electrolyte conditions. Accordingly, we review the use of various polar transition metal sulfur hosts as corresponding solutions to facilitate SRR kinetics at low E/S ratios(< 10 μL mg~(-1)), and the strengths and limitations of different transition metal compounds are presented and discussed from a fundamental perspective. Subsequently, three promising strategies for sulfur hosts that act as anchors and catalysts are proposed to boost lean electrolyte Li–S battery performance. Finally, an outlook is provided to guide future research on high energy density Li–S batteries.展开更多
Short stature is among the most common endocrinological disease phenotypes of childhood and may occur as an isolated finding or in conjunction with other clinical manifestations.Although the diagnostic utility of clin...Short stature is among the most common endocrinological disease phenotypes of childhood and may occur as an isolated finding or in conjunction with other clinical manifestations.Although the diagnostic utility of clinical genetic testing in short stature has been implicated,the genetic architecture and the utility of genomic studies such as exome sequencing(ES)in a sizable cohort of patients with short stature have not been investigated systematically.In this study,we recruited 561 individuals with short stature from two centers in China during a 4-year period.We performed ES for all patients and available parents.All patients were retrospectively divided into two groups:an isolated short stature group(group I,n=257)and an apparently syndromic short stature group(group II,n=304).Causal variants were identified in 135 of 561(24.1%)patients.In group I,29 of 257(11.3%)of the patients were solved by variants in 24 genes.In group II,106 of 304(34.9%)patients were solved by variants in 57 genes.Genes involved in fundamental cellularprocess played an important role in the genetic architecture of syndromic short stature.Distinct genetic architectures and pathophysiological processes underlie isolated and syndromic short stature.展开更多
基金funded by the National Key Research and Development Program of China(No.2022YFB3803600)the National Natural Science Foundation of China(Nos.22368050,22378346)+4 种基金the Key Research and Development Program of Yunnan Province(No.202302AF080002)the Yunnan Basic Applied Research Project(Nos.202401AU070229,202401AT070460)the Scientific Research Fund Project of Yunnan Education Department(Nos.2024J0013,2024J0014)the Open Project of Yunnan Precious Metals Labo-ratory Co.,Ltd(Nos.YPML-2023050259,YPML-2023050260).Au-thors thank the Shiyanjia Lab(www.shiyanjia.com)the Electron Microscopy Center,the Advanced Computing Center,and the Ad-vanced Analysis and Measurement Center of Yunnan University for the sample testing and computational services.
文摘Hydrogen evolution reaction (HER) from water electrolysis is an ideal alternative solution to address the energy crisis and develop clean energy. However, the construction of an efficient electrocatalyst with multiple active sites that can ensure high metal utilization and promote reaction kinetics simultaneously still leaves a major challenge. Herein, we present a facile strategy to synthesize a HER catalyst comprising Pt single atoms (PtSA) anchored in Fe vacancies and Pt quantum dots (Pt_(QD)) on the surface of NiFe LDH. Benefitting from the hierarchical and ultrathin nanosheet arrays and strong electronic interaction between PtSA/Pt_(QD) and NiFe LDH matrix, the optimized sample (Pt_(SA/QD)-NiFe_(V9) LDH) exhibits outstanding HER performance in 1 M KOH with ultra-low overpotentials of 20 and 67 mV at 10 and 100 mA cm^(−2), respectively, outperforming the benchmark Pt/C electrocatalyst. In addition, the electrolyzer using Pt_(SA/QD)-NiFe_(V9) LDH as a cathode requires voltages of only 1.48 and 1.73 V to yield current densities of 10 and 1000 mA cm^(−2), respectively. The combination of in situ tests and density functional theory (DFT) calculations reveal that the synergy of PtSA and Pt_(QD) can optimize the kinetics of water dissociation and hydrogen desorption, thus the Volmer-Tafel pathway prevailing the HER process. This work provides a promising surface engineering strategy to develop catalysts for efficient and robust hydrogen evolution.
基金the technical support for Nano-X from Suzhou Institute of Nano-Tech and NanoBionics,Chinese Academy of Sciences(SINANO)supported by the National Key R&D Program of China(2021YFB3800300)+2 种基金the National Natural Science Foundation of China(22179059,22239002,92372201)the science and technology innovation fund for emission peak and carbon neutrality of Jiangsu province(BK20231512,BK20220034)the Key R&D project funded by department of science and technology of Jiangsu Province(BE2020003)。
文摘Aluminum(Al)exhibits excellent electrical conductivity,mechanical ductility,and good chemical compatibility with high-ionic-conductivity electrolytes.This makes it more suitable as an anode material for all-solid-state lithium batteries(ASSLBs)compared to the overly reactive metallic lithium anode and the mechanically weak silicon anode.This study finds that the pre-lithiated Al anode demonstrates outstanding interfacial stability with the Li_6PS_5Cl(LPSCl)electrolyte,maintaining stable cycling for over 1200 h under conditions of deep charge-discharge.This paper combines the pre-lithiated Al anode with a high-nickel cathode,LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2),paired with the highly ionic conductive LPSCl electrolyte,to design an ASSLB with high energy density and stability.Using anode pre-lithiation techniques,along with dual-reinforcement technology between the electrolyte and the cathode active material,the ASSLB achieves stable cycling for 1000 cycles at a 0.2C rate,with a capacity retention rate of up to 82.2%.At a critical negative-to-positive ratio of 1.1,the battery's specific energy reaches up to 375 Wh kg^(-1),and it maintains over 85.9%of its capacity after 100 charge-discharge cycles.This work provides a new approach and an excellent solution for developing low-cost,high-stability all-solid-state batteries.
基金supported by Multi-Year Research Grants from the University of Macao(MYRG-GRG2023-00010-IAPME,MYRG-GRG2024-00038-IAPME,MYRG2022-00026-IAPME)the Science and Technology Development Fund(FDCT)from Macao SAR(0023/2023/AFJ,0050/2023/RIB2,006/2022/ALC,0087/2024/AFJ,0111/2022/A2).
文摘Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.
基金supported by the Science and Technology Development Fund(FDCT)from Macao SAR(0050/2023/RIB2,0023/2023/AFJ,006/2022/ALC,0111/2022/A2,0105/2023/RIA2)Multi-Year Research Grants(MYRG-GRG2023-00010-IAPME,and MYRG2022-00026-IAPME)from Research&Development Office at University of MacaoShenzhen-Hong Kong-Macao Science and Technology Research Programme(Type C)(SGDX20210823103803017)from Shenzhen.
文摘Large-scale green hydrogen production technology,based on the electrolysis of water powered by renewable energy,relies heavily on non-precious metal oxygen evolution reactions(OER)electrocatalysts with high activity and stability under industrial conditions(6 M KOH,60℃-80℃)at large current density.Here,we construct Fe and Co co-incorporated nickel(oxy)hydroxide(Fe_(2.5)Co_(2.5)Ni_(10)O_(y)H_(z)@NFF)via a multi-metal electrodeposition,which exhibits outstanding OER performance(overpotential:185 mV@10 mA cm^(-2)).Importantly,an overwhelming stability for more than 1100 h at 500 mA cm^(-2)under industrial conditions is achieved.Our combined experimental and computational investigation reveals the surface-reconstructedγ-NiOOH with a high valence state is the active layer,where the optimal(Fe,Co)co-incorporation tunes its electronic structure,changes the potential determining step,and reduces the energy barrier,leading to ultrahigh activity and stability.Our findings demonstrate a facile way to achieve an electrocatalyst with high performance for the industrial production of green hydrogen.
基金funded by the UM’s research funds(MYRG2020-00283-IAPME,MYRG2022-00266-IAPME,and MYRG-GRG2023-00224-IAPME-UMDF)the Science and Technology Development Fund,Macao SAR(FDCT 0006/2021/AKP,FDCT 0096/2020/A2,0013/2021/AMJ,and 0082/2022/A2)City University of Hong Kong(Project No.9020002)
文摘Two-dimensional materials have been widely used to tune the growth and energy-level alignment of perovskites.However,their incomplete passivation and chaotic usage amounts are not conducive to the preparation of highquality perovskite films.Herein,we succeeded in obtaining higher-quality CsPbBr_(3)films by introducing large-area monolayer graphene as a stable physical overlay on top of TiO_(2)substrates.Benefiting from the inert and atomic smooth graphene surface,the CsPbBr_(3)film grown on top by the van der Waal epitaxy has higher crystallinity,improved(100)orientation,and an average domain size of up to 1.22μm.Meanwhile,a strong downward band bending is observed at the graphene/perovskite interface,improving the electron extraction to the electron transport layers(ETL).As a result,perovskite film grown on graphene has lower photoluminescence(PL)intensity,shorter carrier lifetime,and fewer defects.Finally,a photovoltaic device based on epitaxy CsPbBr_(3)film is fabricated,exhibiting power conversion efficiency(PCE)of up to 10.64%and stability over 2000 h in the air.
基金supported by National Nature Science Foundation of China(22379106)Carbon Energy Technology Co.,Ltd.(0501001107)。
文摘We must urgently synthesize highly efficient and stable oxygen-evolution reaction(OER) catalysts for acidic media. Herein, we constructed a series of Ti mesh(TM)-supported RuO_(2)/CoMo_(y)O_(x) catalysts(RuO_(2)/CoMo_(y)O_(x)/TM) with heterogeneous structures. By optimizing the ratio of Co to Mo, RuO_(2)/CoMO_(2)O_(x)/TM with low Ru loading(0.079 mg/cm^(2)) achieves remarkable OER performance(η = 243 mV at 10 mA/cm^(2)) and high stability(300 h @ 10 mA/cm^(2)) in 0.5 mol/L H_(2)SO_(4) electrolyte. The activity of RuO_(2)/CoMo_yO_x/TM can be maintained for 50 h at 100 mA/cm^(2), and a water electrolyzer with RuO_(2)/CoMO_(2)O_(x)/TM as anode can operate for 40 h at 100 mA/cm~2, suggesting the remarkable OER durability of RuO_(2)/CoMo__(y)O__(x)/TM in acidic electrolyte. Owing to the heterogeneous interface between CoMO_(2)O_(x) and RuO_(2), the electronic structure of Ru atoms was optimized and electron-rich Ru was formed. With modulated electronic properties, the dissociation energy of H_(2)O is weakened, and the OER barrier is lowered. This study provides the design of low-cost noble metal catalysts with long-term stability in an acidic environment.
基金supported by the National Natural Science Foundation of China(Grant Nos.12172151 and 12172149).
文摘The relationship between the protective performance of flexible polymer material and material parameters(elasticmodulus,viscosity coefficient)is explored,an impact collision motion equation between two bodies is establishedfrom the viscoelastic material constitutive,and the relationship between the kinematic response and the materialparameters is obtained.Based on the Kelvin constitutive model,a theoretical model for impact between the pro-tective body and the protected body is established,then the dynamic response is obtained.The feasibility of themodel was verified by drop hammer experiment,and the material parameters(elastic modulus,viscosity coeffi-cient)were obtained by formula.The model is discretized and the relationship between local impact response andmaterial parameters is analyzed.The discussion results on the relationship between the impact response and theprotective material performance indicate that adjusting the elastic modulus,viscosity coefficient,and thicknessof the protective material can effectively improve protective effect.
文摘<strong>Background: </strong>Studies have shown that long non-coding RNA (LncRNA) plays a critical role in maintaining genomic instability. The correlation between lncRNA and genomic instability is still worth exploring in bladder cancer as a new tumour marker. <strong>Methods: </strong>Therefore, combined with the lncRNA expression profile and somatic mutation profile of bladder cancer, we established a computing framework of lncRNA related to genomic instability and identified 58 new lncRNA related to genomic instability. Next, we identified a lncRNA signature (GILncSig), based on these 58 new genes, which divided patients into high-risk and low-risk groups. The clinical prognosis was significantly different and was further verified in an independent cohort of patients. <strong>Results: </strong>We confirmed that GILncSig is related to the genomic mutation rate of bladder cancer, suggesting that GILncSig can be used as an indicator of genomic instability. The results show that GILncSig has prognostic value independent of age, sex, grade, and stage and is vital in evaluating clinical prognosis. To sum up, this study provides a vital research basis and methods for further exploring the role of lncRNA in the genomic instability of bladder cancer and provides a theoretical basis for the identification of bladder cancer biomarkers related to genomic instability.
基金Project supported by the National Natural Science Foundation of China(No.51775506)the Zhejiang Provincial Natural Science Foundation of China(No.LY18E050022)+2 种基金the Public Welfare Technology Application Research Project of Zhejiang Province(Nos.LGG19E050022 and 2017C33115)the Zhejiang Provincial Science&Technology Project for Medicine&Health(No.2018KY878)the Open Foundation of Zhejiang Provincial Top Key Discipline of Mechanical Engineering of Hangzhou Dianzi University,China
文摘In maxillofacial surgery, there is a significant need for the design and fabrication of porous scaffolds with customizable bionic structures and mechanical properties suitable for bone tissue engineering. In this paper, we characterize the porous Ti6Al4V implant, which is one of the most promising and attractive biomedical applications due to the similarity of its modulus to human bones. We describe the mechanical properties of this implant, which we suggest is capable of providing important biological functions for bone tissue regeneration. We characterize a novel bionic design and fabrication process for porous implants. A design concept of “reducing dimensions and designing layer by layer” was used to construct layered slice and rod-connected mesh structure (LSRCMS) implants. Porous LSRCMS implants with different parameters and porosities were fabricated by selective laser melting (SLM). Printed samples were evaluated by microstructure characterization, specific mechanical properties were analyzed by mechanical tests, and finite element analysis was used to digitally calculate the stress characteristics of the LSRCMS under loading forces. Our results show that the samples fabricated by SLM had good structure printing quality with reasonable pore sizes. The porosity, pore size, and strut thickness of manufactured samples ranged from (60.95± 0.27)% to (81.23±0.32)%,(480±28) to (685±31)μm, and (263±28) to (265±28)μm, respectively. The compression results show that the Young’s modulus and the yield strength ranged from (2.23±0.03) to (6.36±0.06) GPa and (21.36±0.42) to (122.85±3.85) MPa, respectively. We also show that the Young’s modulus and yield strength of the LSRCMS samples can be predicted by the Gibson-Ashby model. Further, we prove the structural stability of our novel design by finite element analysis. Our results illustrate that our novel SLM-fabricated porous Ti6Al4V scaffolds based on an LSRCMS are a promising material for bone implants, and are potentially applicable to the field of bone defect repair.
基金Supported by the National Key Program of Clinical Science,No.WBYZ 2011-873the Chinese Academy of Medical Sciences Innovation Fund for Medical Sciences,No.2016YFC0901500the Special Research Fund for Central Universities,Peking Union Medical College,No.2017PT31004
文摘BACKGROUND Patients with hypothalamic-pituitary disease have the feature of central obesity,insulin resistance, and dyslipidemia, and there is increased prevalence of liver dysfunction consistent with non-alcoholic fatty liver disease(NAFLD) in this population. The causes of hypopituitarism in the reported studies varied and combined pituitary hormone deficiency including central diabetes insipidus is much common in this population. This retrospective cross-sectional study was performed to analyze the clinical characteristics and related factors with NAFLD and cirrhosis in Chinese adult hypopituitary/panhypopituitary patients.AIM To analyze the clinical characteristics of and related risk factors for NAFLD in Chinese adult hypopituitary patients.METHODS Adult Chinese patients with hypopituitarism and/or panhypopituitarism were enrolled at the Pituitary Center of Peking Union Medical College Hospitalbetween August 2012 and April 2018. According to abdominal ultrasonography,these patients were divided into an NAFLD(-) group and an NAFLD(+) group,and the latter was further divided into an NAFLD group and a cirrhotic group.The data, such as patient characteristics, diagnosis, and treatment, were extracted from medical records, and statistical analysis was performed.RESULTS A total of 36 male and 14 female adult Chinese patients with hypopituitarism were included in this retrospective study; 43(87.0%) of these patients exhibited growth hormone(GH) deficiency, and 39(78.3%) had diabetes insipidus. A total of 27(54.0%) patients were diagnosed with NAFLD, while seven patients were cirrhotic. No significant differences were noted in serum GH or insulin-like growth factor 1 among patients with cirrhosis, subjects with NAFLD, and those without NAFLD. However, plasma osmolality and serum sodium concentration of the cirrhotic patients were 314.9 mOsm/kgH2 O and 151.0 mmol/L,respectively, which were significantly higher than those of the NAFLD patients(P = 0.036 and 0.042, respectively). Overweight/obesity and insulin resistance were common metabolic disorders in this population. The body mass index(BMI)and homeostasis model assessment of insulin resistance parameters of the cirrhotic patients were 27.7 kg/m2 and 9.57, respectively, which were significantly higher than those of the patients without NAFLD(P = 0.011 and0.044, respectively). A correlation analysis was performed, and fasting insulin concentration was positively associated with plasma osmolality in patients with NAFLD, after adjusting for gender, age, and BMI(r = 0.540, P = 0.046), but no correlation was noted in patients without NAFLD.CONCLUSION NAFLD is common in patients with hypopituitarism. Plasma osmolality and serum sodium levels of hypopituitary patients with cirrhosis are higher than those of subjects with NAFLD, and fasting insulin concentration is positively associated with plasma osmolality in patients with NAFLD, which suggests that hyperosmolality might be a contributor to the worsening of NAFLD in hypopituitary patients.
基金supported by the Science and Technology Development Fund from Macao SAR(FDCT)(Nos.0102/2019/A2,0035/2019/AGJ,0154/2019/A3,0081/2019/AMJ,0033/2019/AMJ and 0125/2018/A3)Multi-Year Research Grants(MYRG2018-00003IAPME)from the University of Macao。
文摘Oxygen evolution reaction(OER)is a critical process in electrocatalytic water splitting.However,the development of low-cost,highly efficient OER electrocatalysts by a simple method that can be used for industrial application on a large scale is still a huge challenge.Recently,high entropy alloy(HEA)has acquired extensive attention,which may provide answers to the current dilemma.Here,we report bulk Fe_(50)Mn_(30)Co_(10)Cr_(10),which is prepared by 3D printing on a large scale,as electrocatalyst for OER with high catalytic performance.Especially,an easy approach,corrosion engineering,is adopted for the first time to build an active layer of honeycomb nanostructures on its surface,leading to ultrahigh OER performance with an overpotential of 247 mV to achieve a current density of 10 mA cm^(-2),a low Tafel slope of 63 mV dec^(-1),and excellent stability up to 60 h at 100 mA cm^(-2)in 1 M KOH.The excellent catalytic activity mainly originates from:(1)the binder-free self-supported honeycomb nanostructures and multi-component hydroxides,which improve intrinsic catalytic activity,provide rich active sites,and reduce interfacial resistance;and(2)the diverse valence states for multiple active sites to enhance the OER kinetics.Our findings show that corrosion engineering is a novel strategy to improve the bulk HEA catalytic performance.We expect that this work would open up a new avenue to fabricate large-scale HEA electrocatalysts by 3D printing and corrosion engineering for industrial applications.
基金the Natural Science Foundation of China (22005250)National Key R D Program of China (2022YFB2502000)FWO (12ZV320N)。
文摘The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O_(2) to water(H_2O) or from O_(2) to hydrogen peroxide(H_2O_(2)). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments(e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges.
基金the Research Foundation-Flanders (FWO) for a Research Project (G0B3218N)the financial support by the National Natural Science Foundation of China (22005054)+3 种基金Natural Science Foundation of Fujian Province (2021J01149)State Key Laboratory of Structural Chemistry (20200007)Sichuan Science and Technology Program (project No.: 2022ZYD0016 and 2023JDRC0013)the National Natural Science Foundation of China (project No. 21776120)。
文摘Lithium–sulfur(Li–S) batteries have received widespread attention, and lean electrolyte Li–S batteries have attracted additional interest because of their higher energy densities. This review systematically analyzes the effect of the electrolyte-to-sulfur(E/S) ratios on battery energy density and the challenges for sulfur reduction reactions(SRR) under lean electrolyte conditions. Accordingly, we review the use of various polar transition metal sulfur hosts as corresponding solutions to facilitate SRR kinetics at low E/S ratios(< 10 μL mg~(-1)), and the strengths and limitations of different transition metal compounds are presented and discussed from a fundamental perspective. Subsequently, three promising strategies for sulfur hosts that act as anchors and catalysts are proposed to boost lean electrolyte Li–S battery performance. Finally, an outlook is provided to guide future research on high energy density Li–S batteries.
基金funded in part by the Beijing Natural Science Foundation(JQ20032 to N.W.and to 7191007 to Z.W.)National Natural Science Foundation of China(81822030 and 82072391 to N.W.,81772299and 81930068 to Z.W.,81772301 and 81972132 to G.Q.,81672123and 81972037 to J.Z.)+7 种基金Capital's Funds for Health Improvement and Research(2020-4-40114 to N.W.)Tsinghua University-Peking Union Medical College Hospital Initiative Scientific Research ProgramNational Key Research and Development Program of China(2018YFC0910500 to N.W.and Z.W.,2016YFC0901501 to S.Z.)the PUMC Youth Fund and the Fundamental Research Funds for the Central Universities(3332019052 to Y.M.)the CAMS Initiative Fund for Medical Sciences(2016-I2M-3-003 to G.Q.and N.W.,2016-I2M-2-006 and 2017-I2M-2-001 to Z.W.)the Non-profit Central Research Institute Fund of Chinese Academy of Medical Sciences(2019PT320025 to N.W.)sponsored by GeneScience Pharmaceuticals Co.,Ltd.(Changchun,China)funded by the United States National Institutes of Health(UM1HG006542 and K08 HG008986)。
文摘Short stature is among the most common endocrinological disease phenotypes of childhood and may occur as an isolated finding or in conjunction with other clinical manifestations.Although the diagnostic utility of clinical genetic testing in short stature has been implicated,the genetic architecture and the utility of genomic studies such as exome sequencing(ES)in a sizable cohort of patients with short stature have not been investigated systematically.In this study,we recruited 561 individuals with short stature from two centers in China during a 4-year period.We performed ES for all patients and available parents.All patients were retrospectively divided into two groups:an isolated short stature group(group I,n=257)and an apparently syndromic short stature group(group II,n=304).Causal variants were identified in 135 of 561(24.1%)patients.In group I,29 of 257(11.3%)of the patients were solved by variants in 24 genes.In group II,106 of 304(34.9%)patients were solved by variants in 57 genes.Genes involved in fundamental cellularprocess played an important role in the genetic architecture of syndromic short stature.Distinct genetic architectures and pathophysiological processes underlie isolated and syndromic short stature.
