Synergistic modulation of the d-band center in Ni3S2 by selenium and iron for enhanced oxygen evolution reaction (OER) and urea oxidation reaction (UOR).

Efficient production of green hydrogen energy is crucial in addressing the energy crisis and environmental concerns. The oxygen evolution reaction (OER) poses a challenge in conventional overall water electrolysis due to its slow thermodynamically process. Urea oxidation reaction (UOR) offers an alternative anodic oxidation method that is highly efficient and cost-effective, with favorable thermodynamics and sustainability. Recently, there has been limited research on bifunctional catalysts that exhibit excellent activity for both OER and UOR reactions. In this study, we developed a selenium and iron co-doped nickel sulfide (SeFe-Ni3S2) catalyst that demonstrated excellent Tafel slopes of 53.9 mV dec-1 and 16.4 mV dec-1 for OER and UOR, respectively. Density Functional Theory (DFT) calculations revealed that the introduction of metal (iron) and nonmetallic elements (selenium) was found to coordinate the d-band center, resulting in improved adsorption/desorption energies of the catalysts and reduced the overpotentials and limiting potentials for OER and UOR, respectively. This activity enhancement can be attributed to the altered electronic coordination structure after the introduction of selenium (Se) and iron (Fe), leading to an increase in the intrinsic activity of the catalyst. This work offers a new strategy for bifunctional catalysts for OER and UOR, presenting new possibilities for the future development of hydrogen production and novel energy conversion technologies. It contributes towards the urgent search for technologies that efficiently produce green hydrogen energy, providing potential solutions to mitigate the energy crisis and protect the environment.

Functional MXenes: Progress and Perspectives on Synthetic Strategies and Structure-Property Interplay for Next-Generation Technologies.

MXenes are a class of 2D materials that include layered transition metal carbides, nitrides, and carbonitrides. Since their inception in 2011, they have garnered significant attention due to their diverse compositions, unique structures, and extraordinary properties, such as high specific surface areas and excellent electrical conductivity. This versatility has opened up immense potential in various fields, catalyzing a surge in MXene research and leading to note worthy advancements. This review offers an in-depth overview of the evolution of MXenes over the past 5 years, with an emphasis on synthetic strategies, structure-property relationships, and technological prospects. A classification scheme for MXene structures based on entropy is presented and an updated summary of the elemental constituents of the MXene family is provided, as documented in recent literature. Delving into the microscopic structure and synthesis routes, the intricate structure-property relationships are explored at the nano/micro level that dictate the macroscopic applications of MXenes. Through an extensive review of the latest representative works, the utilization of MXenes in energy, environmental, electronic, and biomedical fields is showcased, offering a glimpse into the current technological bottlenecks, such asstability, scalability, and device integration. Moreover, potential pathways for advancing MXenes toward next-generation technologies are highlighted.

Artificial Photosynthetic System with Spatial Dual Reduction Site Enabling Enhanced Solar Hydrogen Production.

Although S-scheme artificial photosynthesis shows promise for photocatalytic hydrogen production, traditional methods often overly concentrate on a single reduction site. This limitation results in inadequate redox capability and inefficient charge separation, which hampers the efficiency of the photocatalytic hydrogen evolution reaction. To overcome this limitation, a double S-scheme system is proposed that leverages dual reduction sites, thereby preserving energetic photo-electrons and holes to enhance apparent quantum efficiency. The design features a double S-scheme junction consisting of CdS nanospheres decorated with anatase TiO2 nanoparticles coupled with graphitic C3 N4 . The as-prepared catalyst exhibits a hydrogen evolution rate of 26.84 mmol g-1  h-1 and an apparent quantum efficiency of 40.2% at 365 nm. This enhanced photocatalytic hydrogen evolution is ascribed to the efficient charge separation and transport induced by the double S-scheme. Both theoretical calculations and comprehensive spectroscopy tests (both in situ and ex situ) affirm the efficient charge transport across the catalyst interface. Moreover, substituting the reduction-type catalyst CdS with other similar sulfides like ZnIn2 S4 , ZnS, MoS2 and In2 S3 further confirms the feasibility of the proposed double S-scheme configuration. The findings provide a pathway to designing more effective double S-scheme artificial photosynthetic systems, opening up fresh perspectives in enhancing photocatalytic hydrogen evolution performance.

Catalyzing Artificial Photosynthesis with TiO2 Heterostructures and Hybrids: Emerging Trends in a Classical yet Contemporary Photocatalyst.

Titanium dioxide (TiO2 ) stands out as a versatile transition-metal oxide with applications ranging from energy conversion/storage and environmental remediation to sensors and optoelectronics. While extensively researched for these emerging applications, TiO2 has also achieved commercial success in various fields including paints, inks, pharmaceuticals, food additives, and advanced medicine. Thanks to the tunability of their structural, morphological, optical, and electronic characteristics, TiO2 nanomaterials are among the most researched engineering materials. Besides these inherent advantages, the low cost, low toxicity, and biocompatibility of TiO2 nanomaterials position them as a sustainable choice of functional materials for energy conversion. Although TiO2 is a classical photocatalyst well-known for its structural stability and high surface activity, TiO2 -based photocatalysis is still an active area of research particularly in the context of catalyzing artificial photosynthesis. This review provides a comprehensive overview of the latest developments and emerging trends in TiO2 heterostructures and hybrids for artificial photosynthesis. It begins by discussing the common synthesis methods for TiO2 nanomaterials, including hydrothermal synthesis and sol-gel synthesis. It then delves into TiO2 nanomaterials and their photocatalytic mechanisms, highlighting the key advancements that have been made in recent years. The strategies to enhance the photocatalytic efficiency of TiO2 , including surface modification, doping modulation, heterojunction construction, and synergy of composite materials, with a specific emphasis on their applications in artificial photosynthesis, are discussed. TiO2 -based heterostructures and hybrids present exciting opportunities for catalyzing solar fuel production, organic degradation, and CO2 reduction via artificial photosynthesis. This review offers an overview of the latest trends and advancements, while also highlighting the ongoing challenges and prospects for future developments in this classical yet rapidly evolving field.

Enhancing Photocatalytic Hydrogen Evolution by Synergistic Benefits of MXene Cocatalysis and Homo-Interface Engineering.

Photocatalytic water splitting holds great promise as a sustainable and cost-effectiveness alternative for the production of hydrogen. Nevertheless, the practical implementation of this strategy is hindered by suboptimal visible light utilization and sluggish charge carrier dynamics, leading to low yield. MXene is a promising cocatalyst due to its high conductivity, abundance of active sites, tunable terminal functional groups, and great specific surface area. Homo-interface has perfect lattice matching and uniform composition, which are more conducive to photogenerated carriers' separation and migration. In this study, a novel ternary heterogeneous photocatalyst, a-TiO2 /H-TiO2 /Ti3 C2 MXene (MXTi), is presented using an electrostatic self-assembly method. Compared to commercial P25, pristine anatase, and rutile TiO2 , as-prepared MXTi exhibit exceptional photocatalytic hydrogen evolution performance, achieving a rate of 0.387 mmol h-1 . The significant improvement is attributable to the synergistic effect of homo-interface engineering and Ti3 C2 MXene, which leads to widened light absorption and efficient carrier transportation. The findings highlight the potential of interface engineering and MXene cocatalyst loading as a proactive approach to enhance the performance of photocatalytic water splitting, paving the way for more sustainable and efficient hydrogen production.

A Twin S-Scheme Artificial Photosynthetic System with Self-Assembled Heterojunctions Yields Superior Photocatalytic Hydrogen Evolution Rate.

Designing heterojunction photocatalysts imitating natural photosynthetic systems has been a promising approach for photocatalytic hydrogen generation. However, in the traditional Z-Scheme artificial photosynthetic systems, the poor charge separation, and rapid recombination of photogenerated carriers remain a huge bottleneck. To rationally design S-Scheme (i.e., Step scheme) heterojunctions by avoiding the futile charge transport routes is therefore seen as an attractive approach to achieving high hydrogen evolution rates. Herein, a twin S-scheme heterojunction is proposed involving graphitic C3 N4 nanosheets self-assembled with hydrogen-doped rutile TiO2 nanorods and anatase TiO2 nanoparticles. This catalyst shows an excellent photocatalytic hydrogen evolution rate of 62.37 mmol g-1 h-1 and high apparent quantum efficiency of 45.9% at 365 nm. The significant enhancement of photocatalytic performance is attributed to the efficient charge separation and transfer induced by the unique twin S-scheme structure. The charge transfer route in the twin S-scheme is confirmed by in situ X-ray photoelectron spectroscopy (XPS) and electron spin resonance (ESR) spin-trapping tests. Femtosecond transient absorption (fs-TA) spectroscopy, transient-state surface photovoltage (TPV), and other ex situ characterizations further corroborate the efficient charge transport across the catalyst interface. This work offers a new perspective on constructing artificial photosynthetic systems with S-scheme heterojunctions to enhance photocatalytic performance.

Health-adjusted life expectancy (HALE) in Chongqing, China, 2017: An artificial intelligence and big data method estimating the burden of disease at city level.

BACKGROUND: A universally applicable approach that provides standard HALE measurements for different regions has yet to be developed because of the difficulties of health information collection. In this study, we developed a natural language processing (NLP) based HALE estimation approach by using individual-level electronic medical records (EMRs), which made it possible to calculate HALE timely in different temporal or spatial granularities. METHODS: We performed diagnostic concept extraction and normalisation on 13•99 million EMRs with NLP to estimate the prevalence of 254 diseases in WHO Global Burden of Disease Study (GBD). Then, we calculated HALE in Chongqing, 2017, by using the life table technique and Sullivan's method, and analysed the contribution of diseases to the expected years "lost" due to disability (DLE). FINDINGS: Our method identified a life expectancy at birth (LE0) of 77•9 years and health-adjusted life expectancy at birth (HALE0) of 71•7 years for the general Chongqing population of 2017. In particular, the male LE0 and HALE0 were 76•3 years and 68•9 years, respectively, while the female LE0 and HALE0 were 80•0 years and 74•4 years, respectively. Cerebrovascular diseases, cancers, and injuries were the top three deterioration factors, which reduced HALE by 2•67, 2•15, and 1•19 years, respectively. INTERPRETATION: The results demonstrated the feasibility and effectiveness of EMRs-based HALE estimation. Moreover, the method allowed for a potentially transferable framework that facilitated a more convenient comparison of cross-sectional and longitudinal studies on HALE between regions. In summary, this study provided insightful solutions to the global ageing and health problems that the world is facing. FUNDING: National Key R and D Program of China (2018YFC2000400).

Forecasting influenza activity using self-adaptive AI model and multi-source data in Chongqing, China.

BACKGROUND: Early detection of influenza activity followed by timely response is a critical component of preparedness for seasonal influenza epidemic and influenza pandemic. However, most relevant studies were conducted at the regional or national level with regular seasonal influenza trends. There are few feasible strategies to forecast influenza activity at the local level with irregular trends. METHODS: Multi-source electronic data, including historical percentage of influenza-like illness (ILI%), weather data, Baidu search index and Sina Weibo data of Chongqing, China, were collected and integrated into an innovative Self-adaptive AI Model (SAAIM), which was constructed by integrating Seasonal Autoregressive Integrated Moving Average model and XGBoost model using a self-adaptive weight adjustment mechanism. SAAIM was applied to ILI% forecast in Chongqing from 2017 to 2018, of which the performance was compared with three previously available models on forecasting. FINDINGS: ILI% showed an irregular seasonal trend from 2012 to 2018 in Chongqing. Compared with three reference models, SAAIM achieved the best performance on forecasting ILI% of Chongqing with the mean absolute percentage error (MAPE) of 11·9%, 7·5%, and 11·9% during the periods of the year 2014-2016, 2017, and 2018 respectively. Among the three categories of source data, historical influenza activity contributed the most to the forecast accuracy by decreasing the MAPE by 19·6%, 43·1%, and 11·1%, followed by weather information (MAPE reduced by 3·3%, 17·1%, and 2·2%), and Internet-related public sentiment data (MAPE reduced by 1·1%, 0·9%, and 1·3%). INTERPRETATION: Accurate influenza forecast in areas with irregular seasonal influenza trends can be made by SAAIM with multi-source electronic data.

Iodine ion doped bromo bismuth oxide modified bismuth germanate: A direct Z-scheme photocatalyst with enhanced visible-light photocatalytic performance.

A series of Z-scheme I-BiOBr/Bi12GeO20 heterostructures were successfully obtained by a simple method. The Z-scheme I-BiOBr/Bi12GeO20 heterostructures show outstanding photocatalytic performance for degrading the various organic pollutants of the waste water. For degradation of Tetracycline (TC), the Z-scheme 30I-BiOBr/Bi12GeO20 heterostructure exhibits the superior rate constant, which is about 7.73 times, 3.52 times and 1.66 times higher than that of the pure Bi12GeO20, BiOBr and I-BiOBr, respectively. Meanwhile, as we expected, the Z-scheme 30I-BiOBr/Bi12GeO20 heterostructure also displays the enhanced photocatalytic perfomance for degradation of Ciprofloxacin (CIP), 2-Mercaptobenzothiazole (MBT) and reduction of aqueous Cr(VI). The enhancement of photocatalytic performance is attributed to the high redox capacity and the strong interfacial interaction between I-BiOBr and Bi12GeO20, which can effectively improve the separation of photo-induced electron-hole pairs. Additionally, the photocatalytic mechanism over the Z-scheme I-BiOBr/Bi12GeO20 heterostructure is provided. The research work may provide a promising approach to fabricate other Z-scheme heterostructures with efficient photocatalytic performance.

A visible-light-driven Z-scheme CdS/Bi12GeO20 heterostructure with enhanced photocatalytic degradation of various organics and the reduction of aqueous Cr(VI).

A series of Z-scheme CdS/Bi12GeO20 heterostructures were successfully obtained by a simple hydrothermal method. The Z-scheme CdS/Bi12GeO20 heterostructures show outstanding photocatalytic performance for degrading the various organic pollutants of the waste water, and for the reduction of aqueous Cr(VI) under visible light. For degradation of 2-Mercaptobenzothiazole (MBT), the Z-scheme 30CdS/Bi12GeO20 heterostructure exhibits the superior rate constant, which is about 22.67 and 4.6 times higher than that of the pure Bi12GeO20 and CdS, respectively. Meanwhile, as we expected, the Z-scheme 30CdS/Bi12GeO20 heterostructure also displays the enhanced photocatalytic performance for degradation of Levofloxacin (LEV), Ciprofloxacin (CIP), Tetracycline (TC) and reduction of aqueous Cr(VI). The enhancement of photocatalytic performance is attributed to the high redox capacity and the strong interfacial interaction between CdS and Bi12GeO20, which can effectively improve the separation of photo-induced electron-hole pairs. Additionally, the photocatalytic mechanism over the Z-scheme CdS/Bi12GeO20 heterostructure is provided. The research work may provide a promising approach to fabricate other Z-scheme heterostructures with efficient photocatalytic performance.