Rational Integration Research Articles

Modulating the electronic structure of VS2via Ru decoration for an efficient pH-universal electrocatalytic hydrogen evolution reaction.

High-efficiency water electrolysis over a broad pH range is desirable but challenging. Herein, Ru-decorated VS2 on carbon cloth (Ru-VS2/CC) has been in situ synthesized, which features the regulated electronic structure of VS2 by introducing Ru. It is remarkable that the optimal Ru-VS2/CC displays excellent electrocatalytic hydrogen evolution activity with overpotentials of 89 and 87 mV at -10 mA cm-2 in 0.5 M H2SO4 and 1.0 M KOH, respectively. Theoretical calculations and electrocatalytic measurements have demonstrated that introducing Ru induces an enhanced charge density around the Fermi level, facilitating charge transfer and speeding up the electrocatalytic HER kinetics. The Gibbs free energy of the hydrogen intermediate (ΔGH*) of Ru-VS2/CC (0.23 eV) is much closer to zero than that of pure VS2 (0.51 eV) and Ru (-0.37 eV), demonstrating an easier hydrogen adsorption and desorption process for Ru-VS2/CC. The more favorable ΔGH*, differential charge density and the d-band center endow Ru-VS2 with enhanced intrinsic electrocatalytic activity. This study presents a feasible strategy for enhancing electrocatalytic HER activity by the regulation of the electronic structure and the rational integration of dual active components.

Clustering Professional Communication Exploring the Methodology of Clustering the Thematic Dimension in Professional Communication (Politics)

This article examines the challenges associated with selecting appropriate methodologies and principles for organizing the intricate thematic dimension of professional communication. By employing suitable methods, fragmented knowledge can be synthesized, while the explanatory principle facilitates the identification of essential attributes within a given cluster. The rational application and integration of fundamental scientific principles, concepts, and methodological approaches establish specific criteria for objectively evaluating the construct of a cluster. Clustering is recognized as one of the most effective techniques for segmenting the diverse thematic dimensions of professional communication. The article analyzes the “Politics” cluster as an exemplar within the broader thematic dimensions of professional communication. The clustering process within the thematic dimension aims to encompass an expansive scope with a sense of comprehensive coherence. The model for clustering the thematic dimension provides a range ofconstraints and assumptions crucial in creating appropriate constructs.

Heteroatom-Coordinated Palladium Molecular Catalysts for Sustainable Electrochemical Production of Hydrogen Peroxide.

Currently, hydrogen peroxide (H2O2) manufacturing involves an energy-intensive anthraquinone technique that demands expensive solvent extraction and a multistep process with substantial energy consumption. In this work, we synthesized Pd-N4-CO, Pd-S4-NCO, and Pd-N2O2-C single-atom catalysts via an in situ synthesis approach involving heteroatom-rich ligands and activated carbon under mild reaction conditions. It reveals that palladium atoms interact strongly with heteroatom-rich ligands, which provide well-defined and uniform active sites for oxygen (O2) electrochemically reduced to hydrogen peroxide. Interestingly, the Pd-N4-CO electrocatalyst shows excellent performance for the electrocatalytic reduction of O2 to H2O2 via a two-electron transfer process in a base electrolyte, exhibiting a negligible amount of onset overpotential and >95% selectivity within a wide range of applied potentials. The electrocatalysts based on the activity and selectivity toward 2e- ORR follow the order Pd-N4-CO > Pd-N2O2-C > Pd-S4-NCO in agreement with the pull-push mechanism, which is the Pd center strongly coordinated with high electronegativity donor atoms (N and O atoms) and weakly coordinated with the intermediate *OOH to excellent selectivity and sustainable production of H2O2. According to density functional theory, Pd-N4 is the active site for selectivity toward H2O2 generation. This work provides an emerging technique for designing high-performance H2O2 electrosynthesis catalysts and the rational integration of several active sites for green and sustainable chemical synthesis via electrochemical processes.

Design of Traffic Improvement Plan for Line 1 Baijiahu Station of Nanjing Metro

The article proposes design improvements for the current issues at Baijiahu Station, reorganizing the layout of surrounding transportation facilities to address the existing disorder. Based on an understanding of Baijiahu Metro Station, the article analyzes the regional conditions, target service users, and potential future service users. Through on-site inspections and predictions based on current pedestrian flow data and conditions, the article forecasts the future demand for various transportation modes at Baijiahu Station. Subsequently, it puts forward improvement measures and plans concerning the layout of public facilities around Baijiahu Metro Station, the integration of subway and surface transportation, and crowd organization. These proposals aim to provide feasible planning solutions for the reconstruction and future development of Baijiahu Metro Station. Finally, the article uses simulation software to compare the effects before and after the improvements. This allows the optimized plan to effectively enhance the service efficiency and quality of the metro station, facilitating the rational integration of the subway into urban transportation and thereby improving the city's public transportation capacity and service standards.

Empirical study on the impact of digital economy on carbon emission intensity--based on the mediating role of technological innovation

With the proposal of “Carbon Peak and Carbon Neutrality” goals, China is facing a more serious carbon emissions reduction situation, and how the booming digital economy effectively helps China’s carbon emissions reduction is one of the most urgent things that should be solved. To study the impact of the digital economy on carbon emission intensity, this paper is based on the panel data of 30 provinces in China (excluding Tibet, Hong Kong, Macao, and Taiwan) from 2011 to 2021, and applies the double-fixed effect model and the threshold effect model to study the impact of the digital economy on carbon emission intensity and the mechanism of its action, as well as to analyze the mechanism of the digital economy’s action on carbon emission intensity from the perspective of technological innovation. The results of the study show that: i) The digital economy can reduce the intensity of regional carbon emissions; ii) The carbon emission reduction effect of the digital economy is non-linear, and its carbon emission reduction effect gradually increases with the level of development of the digital economy; iii) In addition to the direct impact of the digital economy on carbon emission intensity, it also has an indirect impact on carbon emissions through technological innovation; iv) There is regional heterogeneity in the carbon emission reduction effect of the digital economy, and the carbon emission reduction effect is more significant in the central and western parts of the country and regions with a high level of human capital development. Based on the conclusions obtained, this paper suggests: i) The rational integration of the digital economy and regional development should be strengthened; ii) Strong provinces in the digital economy should be encouraged to help weaker provinces, to narrow the “digital divide” between provinces; iii) Differentiated development strategies should be formulated in accordance with local conditions, to give full play to the optimal effect of the digital economy in carbon emission reduction.

Single or pluralistic? The game and balance of China's community governance policy tools.

Policy tools embody policy concepts and are essential to achieving policy objectives. The effective allocation of policy tools directly impacts the effectiveness of community governance and determines the modernization process of grassroots governance. We aim to analyze the logic of community governance policy tool selection, and then provide assistance for the modernization of grassroots governance. We selected 100 national and provincial government work reports and 63 policy documents related to community governance during China's "12th Five-Year Plan" to "14th Five-Year Plan" period as analysis samples. And build an analysis framework based on the three dimensions of time, space, and tools. We used Nvivo.20 software for text encoding analysis. Based on the model framework, we analyze the results as follows. From the perspective of the time dimension, among the five types of policy tools, the proportion of command-type policy tools used showed a downward trend, from 88.16% in the 12th Five-Year Plan to 83.50% in the 14th Five-Year Plan. However, motivation-type and persuasion-type tools showed an upward trend, rising from 1.34% and 5.26% in the 12th Five-Year Plan period to 3.40% and 8.74% in the 14th Five-Year Plan respectively. The system-change-type policy tools decreased from 1.32% in the 12th Five-Year Plan to 0.97% in the 14th Five-Year Plan. The proportion of capacity-building-type policy tools has gradually increased from 2.63% in the 12th Five-Year Plan to 4.85% in the 14th Five-Year Plan. From the perspective of spatial dimension, apart from command and persuasion policy tools, the usage frequency of the other three types of policy tools in the three major regions all display a "growth-decline-growth" trend. From the perspective of tool dimension, command-type policy tools are dominant in China's community governance, with a cumulative frequency of 1405 times and a high proportion of 81.75%. Apart from command policy tools, persuasive policy tools and capacity-building policy tools have a relatively high proportion, with usage frequencies of 186 and 78 respectively. We found that current community governance policy tools mainly consist of command tools. However, there is a trend towards combining tools such as command, persuasion, incentive, capacity building, and system change in the future. There is a typical contradiction between instrumental rationality and value rationality, indicating an evolution from instrumental rationality to the integration of instrumental and value rationality. This study addresses the conflict of policy tools through rational guidance of values, the rational guarantee of tools, and cooperation to achieve the goal of high-quality development of community governance.

Artificial photosynthetic cells with biotic–abiotic hybrid energy modules for customized CO2 conversion

Programmable artificial photosynthetic cell is the ultimate goal for mimicking natural photosynthesis, offering tunable product selectivity via reductase selection toward device integration. However, this concept is limited by the capacity of regenerating the multiple cofactors that hold the key to various reductases. Here, we report the design of artificial photosynthetic cells using biotic–abiotic thylakoid–CdTe as hybrid energy modules. The rational integration of thylakoid with CdTe quantum dots substantially enhances the regeneration of bioactive NADPH, NADH and ATP cofactors without external supplements by promoting proton-coupled electron transfer. Particularly, this approach turns thylakoid highly active for NADH regeneration, providing a more versatile platform for programming artificial photosynthetic cells. Such artificial photosynthetic cells can be programmed by coupling with diverse reductases, such as formate dehydrogenase and remodeled nitrogenase for highly selective production of formate or methane, respectively. This work opens an avenue for customizing artificial photosynthetic cells toward multifarious demands for CO2 conversion.

Rational Integration of SnMOF/SnO2 Hybrid on TiO2 Nanotube Arrays: An Effective Strategy for Accelerating Formaldehyde Sensing Performance at Room Temperature.

Formaldehyde is ubiquitously found in the environment, meaning that real-time monitoring of formaldehyde, particularly indoors, can have a significant impact on human health. However, the performance of commercially available interdigital electrode-based sensors is a compromise between active material loading and steric hindrance. In this work, a spaced TiO2 nanotube array (NTA) was exploited as a scaffold and electron collector in a formaldehyde sensor for the first time. A Sn-based metal-organic framework was successfully decorated on the inside and outside of TiO2 nanotube walls by a facile solvothermal decoration strategy. This was followed by regulated calcination, which successfully integrated the preconcentration effect of a porous Sn-based metal-organic framework (SnMOF) structure and highly active SnO2 nanocrystals into the spaced TiO2 NTA to form a Schottky heterojunction-type gas sensor. This SnMOF/SnO2@TiO2 NTA sensor achieved a high room-temperature formaldehyde response (1.7 at 6 ppm) with a fast response (4.0 s) and recovery (2.5 s) times. This work provides a new platform for preparing alternatives to interdigital electrode-based sensors and offers an effective strategy for achieving target preconcentrations for gas sensing processes. The as-prepared SnMOF/SnO2@TiO2 NTA sensor demonstrated excellent sensitivity, stability, reproducibility, flexibility, and convenience, showing excellent potential as a miniaturized device for medical diagnosis, environmental monitoring, and other intelligent sensing systems.

Defects-enriched two-dimensional ultrathin g-C3N4/In2O3 nanoparticles for effective NO2 detection at room temperature

Rational integration of ultrathin two-dimensional(2D) graphitic carbon nitride(g-C3N4) nanosheets and indium oxide(In2O3) nanoparticles was implemented by hydrothermal and calcination. The optimized composites demonstrated an outstanding NO2 response of 1470 (5 ppm) and short response/recovery time (67/46 s). Moreover, the prepared composites displayed excellent reproducibility, low detection limit (18 ppb), and satisfactory selectivity to NO2 at room temperature (RT). The gas sensing mechanism was also proposed and verified by the density functional theory calculation. The outstanding gas sensing properties might be due to the combination of heterojunction, enhanced specific surface, and enriched defects. This study gives a reference for designing sensing materials by forming heterojunctions between metal oxides and g-C3N4 for superior gas sensitivity and exploring the manufacture of advanced gas sensors.

Bimetallic CoCu nanoparticles anchored on COF/SWCNT for electrochemical detection of carbendazim

Carbendazim (CBZ) is a widespread fungicide used in crop protection, but the CBZ residues in drinking water, fruits, and vegetables can also cause adverse impacts on public health due to direct exposure. In this paper, a ternary synergistic composite of bimetallic CoCu nanoparticles anchored on covalent organic framework/single-walled carbon nanotube (CoCu/COF/SWCNT) was prepared and further applied as an electrochemical sensing platform for detecting CBZ. The sensor showed a sensitive response performance toward CBZ oxidation, as a result of the enhanced charge transfer ability, large electrochemically active surface area, and high electro-catalytic activity from the rational integration of the ternary components in CoCu/COF/SWCNT. Under the optimal conditions, the proposed sensor exhibited a detection range of 0.001 to 10 μM and a limit detection of 0.65 nM for CBZ detection. In addition, the sensor displayed practical feasibility for the determination of CBZ in water and pear samples with a recovery of 96.1 % to 102.1 %.

Cobalt phosphide integrated manganese-doped metallic 1T-vanadium disulfide: Unveiling a 2D-2D tangled 3D heterostructure for robust water splitting

The rational integration of a 2D layered transition metal sulfide and phosphide in a single heterostructure can bring a breakthrough to produce hydrogen through controlled manipulation of electronic structure. Here, we report a novel design of a hierarchical 2D−2D tangled 3D heterostructure of manganese-doped 1T vanadium disulfide (1T−Mn−VS2), assembled with cobalt phosphide (Co2P), at the flexible carbon cloth as 1T−Mn−VS2@Co2P@CC. The HER active 1T−Mn−VS2 bearing catalytically active edge sites, with numbers of basal planes and OER active Co2P, create synergism and hastening rection kinetics towards bifunctional water splitting. The heterostructure display significantly low over potential of 98 and 250 mV for HER and OER at 10 mA cm−2. The 1T−Mn−VS2@Co2P@CC (+,-) electrochemical cell needs 1.50 V to reach a current density of 10 mAcm−2. The implication of defect engineering along with interface modeling validated by DFT study, induces the regulation of electronic structure for fast redistribution of local charges/electron transfer.

Anchoring Bi2S3 quantum dots on flower-like TiO2 nanostructures to boost photoredox coupling of H2 evolution and oxidative organic transformation

The rational integration of semiconductor quantum dots (QDs) with anatase TiO2 nanostructures is a promising strategy to develop efficient photocatalysts. Herein, Bi2S3QD/TiO2 photocatalyst was constructed by controllably depositing Bi2S3 QDs on flower-like TiO2 nanostructures and used for the photocatalytic redox-coupling reaction of H2 evolution and oxidative transformation of benzyl alcohol. The abundant amino groups in TiO2 nanostructures served as the anchoring sites for uniform growth of Bi2S3 QDs. The anchoring of Bi2S3 QDs onto TiO2 nanostructures not only enhanced the photoabsorption ability and the photogenerated charge separation efficiency but also afforded powerful photogenerated charge carriers and abundant active sites for the photocatalytic reaction. As a result, the Bi2S3QD/TiO2 photocatalyst exhibited a favorable performance in the redox-coupling reaction, providing the high production rates of H2 up to 4.75 mmol·gcat−1·h−1 and benzaldehyde up to 6.12 mmol·gcat−1·h−1, respectively, as well as an excellent stability in the long-term photocatalytic reaction. Meanwhile, a trace amount of water in the reaction system could act as a promoter to accelerate the photocatalytic redox-coupling reaction. The photocatalytic mechanism following S-scheme heterojunction was proposed according to the systematic characterizations and experimental results. This work offers some insight into the rational construction of efficient and cost-effective photocatalysts for the conversion of solar to chemical energy.

On the Rational Integrals of Two-Dimensional Natural Systems

On the Rational Integrals of Two-Dimensional Natural Systems

Synergistic Dual-Mechanism Localized Heat Channeling and Spectrum-Tailored Liquid Metal Hydrogels for Efficient Solar Water Evaporation and Desalination.

Photothermal hydrogels featuring broadband light absorption abilities and highly hydrated networks provide an appealing mass-energy transfer platform for water evaporation by using solar energy. However, the targeted delivery of solar heat energy to power the water evaporation process remains challenging. Herein, enlightened by metal-phenolic coordination chemistry and camouflaged architecture, photothermal hydrogels with dual-mechanism vaporization structure are tactfully designed via a rational interfacial engineering and integration strategy to enable near-µm heat confinement and highly efficient light-to-heat conversion ability. The spectrum-tailored liquid metal droplet (LMGAs-FeIII ) and optimized carbon-wrapped silver nanowire sponge (Ag@C750 ) are integrally built as photothermal promotors/channels and jointly embedded into a highly hydratable poly(vinyl alcohol) hydrogel, denoted as PALGH,to synergisticallyboost watermolecule activation and interfacial vaporization behavior by triggering robust photothermal performance. As a result, under one sun irradiation, the all-embracing PALGH hydrogel evaporation system achieves a brine evaporation rate to a high level of 3.47kg m-2 h-1 , and >19 L m-2 clean water of PALGH is ideally delivered daily when purifying natural seawater. This work offers not only a rational design principle to create sophisticated photothermal materials but also replenishes insight into solar heat generation and water transportation in a cross-media system.

An Organodiselenide Comediator to Facilitate Sulfur Redox Kinetics in Lithium-Sulfur Batteries with Encapsulating Lithium Polysulfide Electrolyte.

Lithium-sulfur (Li-S) batteries are regarded as promising high-energy-density energy storage devices. However, the cycling stability of Li-S batteries is restricted by the parasitic reactions between Li metal anodes and soluble lithium polysulfides (LiPSs). Encapsulating LiPS electrolyte (EPSE) can efficiently suppress the parasitic reactions but inevitably sacrifices the cathode sulfur redox kinetics. To address the above dilemma, a redox comediation strategy for EPSE is proposed to realize high-energy-density and long-cycling Li-S batteries. Concretely, dimethyl diselenide (DMDSe) is employed as an efficient redox comediator to facilitate the sulfur redox kinetics in Li-S batteries with EPSE. DMDSe enhances the liquid-liquid and liquid-solid conversion kinetics of LiPS in EPSE while maintains the ability to alleviate the anode parasitic reactions from LiPSs. Consequently, a Li-S pouch cell with a high energy density of 359 Wh kg-1 at cell level and stable 37 cycles is realized. This work provides an effective redox comediation strategy for EPSE to simultaneously achieve high energy density and long cycling stability in Li-S batteries and inspires rational integration of multi-strategies for practical working batteries.

An Organodiselenide Comediator to Facilitate Sulfur Redox Kinetics in Lithium–Sulfur Batteries with Encapsulating Lithium Polysulfide Electrolyte

AbstractLithium–sulfur (Li–S) batteries are regarded as promising high‐energy‐density energy storage devices. However, the cycling stability of Li–S batteries is restricted by the parasitic reactions between Li metal anodes and soluble lithium polysulfides (LiPSs). Encapsulating LiPS electrolyte (EPSE) can efficiently suppress the parasitic reactions but inevitably sacrifices the cathode sulfur redox kinetics. To address the above dilemma, a redox comediation strategy for EPSE is proposed to realize high‐energy‐density and long‐cycling Li–S batteries. Concretely, dimethyl diselenide (DMDSe) is employed as an efficient redox comediator to facilitate the sulfur redox kinetics in Li–S batteries with EPSE. DMDSe enhances the liquid–liquid and liquid–solid conversion kinetics of LiPS in EPSE while maintains the ability to alleviate the anode parasitic reactions from LiPSs. Consequently, a Li–S pouch cell with a high energy density of 359 Wh kg−1 at cell level and stable 37 cycles is realized. This work provides an effective redox comediation strategy for EPSE to simultaneously achieve high energy density and long cycling stability in Li–S batteries and inspires rational integration of multi‐strategies for practical working batteries.

Green synthesis of stable hybrid biocatalyst using a hydrogen-bonded, π-π-stacking supramolecular assembly for electrochemical immunosensor

Rational integration of native enzymes and nanoscaffold is an efficient means to access robust biocatalyst, yet remains on-going challenges due to the trade-off between fragile enzymes and harsh assembling conditions. Here, we report a supramolecular strategy enabling the in situ fusion of fragile enzymes into a robust porous crystal. A c2-symmetric pyrene tecton with four formic acid arms is utilized as the building block to engineer this hybrid biocatalyst. The decorated formic acid arms afford the pyrene tectons high dispersibility in minute amount of organic solvent, and permit the hydrogen-bonded linkage of discrete pyrene tectons to an extended supramolecular network around an enzyme in almost organic solvent-free aqueous solution. This hybrid biocatalyst is covered by long-range ordered pore channels, which can serve as the gating to sieve the catalytic substrate and thus enhance the biocatalytic selectivity. Given the structural integration, a supramolecular biocatalyst-based electrochemical immunosensor is developed, enabling the pg/mL detection of cancer biomarker.

A Smart Active Phase-Change Micropump Based on CMOS-MEMS Technology.

The rational integration of many microfluidic chips and micropumps remains challenging. Due to the integration of the control system and sensors in active micropumps, they have unique advantages over passive micropumps when integrated into microfluidic chips. An active phase-change micropump based on complementary metal-oxide-semiconductor-microelectromechanical system (CMOS-MEMS) technology was fabricated and studied theoretically and experimentally. The micropump structure is simple and consists of a microchannel, a series of heater elements along the microchannel, an on-chip control system, and sensors. A simplified model was established to analyze the pumping effect of the traveling phase transition in the microchannel. The relationship between pumping conditions and flow rate was examined. Based on the experimental results, the maximum flow rate of the active phase-change micropump at room temperature is 22 µL/min, and long-term stable operation can be achieved by optimizing heating conditions.

Pedagogical conditions for the use of electronic educational resources in the context of the modernization of linguistic education

The aim of this paper is to analyze the main parameters of electronic educational resources (EER) in foreign language education at university level, and to identify the pedagogical conditions for their optimal use with the final goal of motivation of students for learning activities and as a result the quality of education and optimizing language training. Using theoretical methods, data were obtained on the current trends in the use of electronic educational resources in the study of foreign languages; оn the basis of systematic observations of the students’ activity in the classroom and the evaluation of their productive activities, pedagogical conditions were identified and justified that contribute to the activity of students when working with EER, taking into account the purpose of these resources. The identified pedagogical conditions for the use of EER in the educational process, according to the intended purpose of these resources and taking into account the peculiarities of perception and the needs of modern students, contribute to a more rational integration of EER in teaching students foreign languages, the optimal use of these resources to motivate students to study and increase the productivity of the educational process. Some of the conclusions reached are that EERs have a significant potential for intensifying the educational process, provided that the identified pedagogical conditions for their use are met. These conditions relate to the objectives of a particular stage of learning, taking into account the cognitive characteristics of students, the possibility of choosing and determining the relevant information by them, the interactive nature of computer tasks. The increase of the open tasks in the educational process and multimedia resources are intended to orient the teacher in the choice of the necessary EER and the methodology for its application.

Assembling Amorphous Metal–Organic Frameworks onto Heteroatom‐Doped Carbon Spheres for Remarkable Bifunctional Oxygen Electrocatalysis

AbstractMultifunctional electrocatalysts play an increasingly crucial role in various practical electrochemical energy conversion devices. Especially, on the air cathode of rechargeable zinc–air batteries (ZABs), oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), requiring efficient bifunctional electrocatalysts, are switched during discharging and charging process. Here, supported by the theoretical computations, a facile strategy for the in situ assembly of NiFe‐MOFs nanosheets on heteroatoms‐doped porous activated carbon spheres is developed. The newly designed electrocatalyst (NP‐ACSs@NiFe‐MOFs) shows excellent performance toward bifunctional oxygen electrocatalysis. Specifically, a remarkable low value of potential gap (ΔE= 0.61 V), which is the difference between the potential to reach an OER current density of 10 mA cm−2and ORR half‐wave potential, is achieved in 0.1 mKOH. Notably, the aqueous ZAB based on NP‐ACSs@NiFe‐MOFs shows super cycle stability with small voltage gap of only 0.79 V when cycled for 450 h at 10 mA cm−2. Also, the quasi‐solid‐state ZAB indicates excellent flexibility and cycling stability. This study presents a facile strategy for the rational integration of different catalytically active components, and can be extended to prepare other strongly competitive multifunctional electrocatalysts.