Assessing the Charge Carrier Dynamics at Hybrid Interfaces of Organic Photoanodes for Solar Fuels.

Organic semiconductors (OSCs) have emerged as promising active layers for photoanodes to drive photoelectrochemical (PEC) oxidation reactions. Interfacing an OSC with an inorganic electron transport layer (ETL) is key to enabling both high performance and stability. While spectroelectrochemical techniques have been established for the evaluation of inorganic interfaces, allowing rational optimization toward higher performances, a similar level of understanding for hybrid organic-inorganic interfaces remains elusive. To close this knowledge gap, we first perform a systematic parameter study (ETL thickness, potential dependency, and light intensity) on a state-of-the-art organic photoanode to establish factors determining the photoelectrochemical impedance spectroscopy (PEIS) response. Coupled with in situ UV-Vis characterizations, key charge transfer processes are clearly assigned to the PEIS features.

APPROACH: Sensitive Detection of Exosomal Biomarkers by Aptamer-Mediated Proximity Ligation Assay and Time-Resolved Förster Resonance Energy Transfer.

Exosomal biomarker detection holds great importance in the field of in vitro diagnostics, offering a non-invasive and highly sensitive approach for early disease detection and personalized treatment. Here, we proposed an "APPROACH" strategy, combining aptamer-mediated proximity ligation assay (PLA) with rolling circle amplification (RCA) and time-resolved Förster resonance energy transfer (TR-FRET) for the sensitive and semi-homogenous detection of exosomal biomarkers. PLA probes consisted of a cholesterol-conjugated oligonucleotide, which anchored to the membrane of an exosome, and a specific aptamer oligonucleotide that recognized a target protein of the exosome; the proximal binding of pairs of PLA probes to the same exosome positioned the oligonucleotides in the vicinity of each other, guiding the hybridization and ligation of two subsequently added backbone and connector oligonucleotides to form a circular DNA molecule. Circular DNA formed from PLA underwent rolling circle amplification (RCA) for signal amplification, and the resulting RCA products were subsequently quantified by TR-FRET. The limits of detection provided by APPROACH for the exosomal biomarkers CD63, PD-L1, and HER2 were 0.46 ng∙µL-1, 0.77 ng∙µL-1, and 1.1 ng∙µL-1, respectively, demonstrating excellent analytical performance with high sensitivity and quantification accuracy. Furthermore, the strategy afforded sensitive detection of exosomal CD63 with a LOD of 1.56 ng∙µL-1 in complex biological matrices, which underscored its anti-interference capability and potential for in vitro detection. The proposed strategy demonstrates wide-ranging applicability in quantifying diverse exosomal biomarkers while exhibiting robust analytical characteristics, including high sensitivity and accuracy.

Electrostatic [FeFe]-hydrogenase-carbon nitride assemblies for efficient solar hydrogen production.

The assembly of semiconductors as light absorbers and enzymes as redox catalysts offers a promising approach for sustainable chemical synthesis driven by light. However, achieving the rational design of such semi-artificial systems requires a comprehensive understanding of the abiotic-biotic interface, which poses significant challenges. In this study, we demonstrate an electrostatic interaction strategy to interface negatively charged cyanamide modified graphitic carbon nitride (NCNCNX) with an [FeFe]-hydrogenase possessing a positive surface charge around the distal FeS cluster responsible for electron uptake into the enzyme. The strong electrostatic attraction enables efficient solar hydrogen (H2) production via direct interfacial electron transfer (DET), achieving a turnover frequency (TOF) of 18 669 h-1 (4 h) and a turnover number (TON) of 198 125 (24 h). Interfacial characterizations, including quartz crystal microbalance (QCM), photoelectrochemical impedance spectroscopy (PEIS), intensity-modulated photovoltage spectroscopy (IMVS), and transient photocurrent spectroscopy (TPC) have been conducted on the semi-artificial carbon nitride-enzyme system to provide a comprehensive understanding for the future development of photocatalytic hybrid assemblies.

Synergizing economic growth and carbon emission reduction in China: A path to coupling the MFLP and PLUS models for optimizing the territorial spatial functional pattern.

Carbon emissions caused by economic growth are the main cause of global warming, but controlling economic growth to reduce carbon emissions does not meet China's conditions. Therefore, how to synergize economic growth and carbon emission reduction is not only a sustainable development issue for China, but also significant for mitigating global warming. The territorial spatial functional pattern (TSFP) is the spatial carrier for coordinating economic development and carbon emissions, but how to establish the TSFP of synergizing economic growth and carbon emission reduction remains unresolved. We propose a decision framework for optimizing TSFP coupled with the multi-objective fuzzy linear programming and the patch-generating land use simulation model, to provide a new path to synergize economic growth and carbon emission reduction in China. To confirm the reliability, we took Qionglai City as the demonstration. The results found a significant spatiotemporal coupling between TSFP and the synergistic states between economic growth and carbon emission reduction (q ≥ 0.8220), which resolves the theoretical uncertainty about synergizing economic growth and carbon emission reduction through the path of TSFP optimization. The urban space of Qionglai City in 2025 and 2030 obtained by the decision framework was 6497.57 hm2 and 6628.72 hm2 respectively, distributed in the central and eastern regions; the rural space was 60,132.92 hm2 and 56,084.97 hm2, concentrated in the east, with a few located in the west; and the ecological space was 71,072.52 hm2 and 74,998.31 hm2, mainly located in the western and southeastern areas. Compared with the TSFP in 2020, the carbon emission intensity of the TSFP obtained by the decision framework was reduced by 0.7 and 4.7 tons/million yuan, respectively, and realized the synergy between economic growth and carbon emission reduction (decoupling index was 0.25 and 0.21). Further confirming that TSFP optimization is an effective way to synergize economic growth and carbon emission reduction, which can provide policy implications for coordinating economic growth and carbon emissions for China and even similar developing countries.