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Incompetent perforator veins (IPVs) are a critical driver of refractory venous leg ulcers (VLUs). Guideline-endorsed endovenous thermal ablation techniques face substantial implementation barriers due to high device costs and incompatibility with value-based payment models, creating a significant treatment gap. This report introduces Percutaneous Ablation of Perforator Veins using Electrocoagulation (PAPS-PEC)-a novel adaptation of the PAPS principle that leverages ubiquitous electrosurgical equipment to offer a safe, effective, and economically sustainable solution. We present PAPS-PEC application in a 68-year-old male with a recurrent VLU (30×50 mm, CEAP C6) subtended by two IPVs. The office-based procedure was performed under local anesthesia. An 18-gauge electrosurgical needle was guided into each IPV to deliver targeted direct-current energy (10 W, 15 s per quadrant), achieving immediate occlusion confirmed by intraprocedural sonography. The procedure was well-tolerated with no adverse events. Complete ulcer re-epithelialization was achieved at 3 months. At one year, duplex ultrasound confirmed sustained IPV occlusion with no ulcer recurrence. The patient's clinical status improved markedly, with the Venous Clinical Severity Score (VCSS) decreasing from 14 to 4 and the CIVIQ-14 score from 50 to 22. PAPS-PEC is a safe, effective, and exceptionally cost-effective office-based modality for treating IPV-related VLUs. By repurposing existing technology, it directly addresses the economic and accessibility barriers of current standards. These promising findings warrant larger prospective studies to validate its role as a standard-of-care option in managing advanced chronic venous insufficiency, especially in resource-constrained settings. Venous leg ulcers are chronic wounds that heal slowly, often caused by underlying faulty veins known as incompetent perforator veins (IPVs). While standard treatments like laser or radiofrequency ablation are effective, their high cost creates significant barriers for many patients, particularly within healthcare systems that have strict budget controls. This report introduces a new, highly cost-effective technique called Percutaneous Ablation of Perforator Veins using Electrocoagulation (PAPS-PEC). This method utilizes a standard, widely available electrosurgical needle to precisely close these faulty veins. We successfully applied this technique to a 68-year-old man with a non-healing ulcer. The procedure was quick, safe, and performed conveniently in an office setting. His ulcer healed completely, and he remained free of recurrence five years later. PAPS-PEC shows great promise in making advanced vein care both affordable and accessible to a much larger global population, offering a practical and sustainable solution to a common and debilitating health problem.
Growing public environmental concern (PEC) has increasingly shaped the governance of agricultural sustainability, yet its role in mitigating agricultural carbon emissions (ACE) remains insufficiently understood. This study contributes to the literature by incorporating informal environmental regulation into the analysis of ACE and developing an integrated PEC-GTI-ACE analytical framework. Using panel data from 30 Chinese provinces over 2011-2022, we examine how PEC affects agricultural carbon emission intensity, as well as the moderating and nonlinear roles of green technological innovation (GTI), employing two-way fixed effects, moderation, and threshold regression models. The empirical results show that higher levels of public environmental concern significantly reduce agricultural carbon emission intensity, with a stable and robust coefficient of approximately - 0.060 across alternative specifications. GTI plays a reinforcing role in this process. The interaction between public concern and green innovation is significantly negative, with an estimated coefficient of - 0.014, indicating that advances in green innovation amplify the carbon mitigation effect of PEC. Further analysis reveals a nonlinear threshold effect in GTI, with a single threshold estimated at 0.337. Once this threshold is exceeded, the suppressive impact of PEC on ACE becomes markedly stronger. Subregional analyses indicate that the threshold effects observed in the eastern and central regions are broadly consistent with the national pattern, while the western region exhibits pronounced heterogeneity. By uncovering both the complementary and threshold-based mechanisms between public environmental awareness and green technological innovation, this study provides new evidence on how behavioral and technological factors jointly shape agricultural carbon reduction. Overall, the findings suggest that PEC and GTI act as complementary forces in mitigating ACE.
Sensitive and precise detection of prostate-specific antigen (PSA) is essential for the early diagnosis and monitoring of prostate cancer. However, conventional detection methods often suffer from limited sensitivity, poor selectivity, highlighting the need for advanced sensing platforms. Photoelectrochemical (PEC) biosensing achieve for PSA accurate detection due to its high sensitivity, low background noise, and simplicity. Nonetheless, enhancing light absorption and charge separation efficiency remains a major challenge. In this study, we addressed this challenge by modulating the emission wavelength of carbon dots (CDs) and integrating them into a TiO2/In2S3-based heterojunction. Three types of CDs, including blue, green and red-emitting CDs (B-CDs, G-CDs, and R-CDs) were synthesized via a hydrothermal method and systematically optimized for photophysical and electronic performance. Among them, R-CDs exhibited superior visible-light absorption, enhanced electron transport, and abundant surface functional groups. When incorporated into a TiO2/In2S3 composite, R-CDs significantly boosted the photocurrent response (-112 μA), outperforming the B-CDs (-60 μA) and G-CDs (-88 μA) counterparts. Comprehensive characterizations confirmed the formation of a well-integrated ternary heterojunction with efficient charge separation and reactive oxygen species (ROS) generation. A PEC aptasensor was subsequently developed based on the optimized TiO2/In2S3/R-CDs photoelectrode for PSA detection. The sensor demonstrated a wide linear detection range (0.002-100 ng/mL), an ultralow detection limit (5.0 pg/mL), and excellent selectivity. It also exhibited strong stability and reproducibility, with recovery rates of 96.6-100.4% in spiked serum samples. This study not only presents a highly sensitive PEC platform for clinical diagnostics but also underscores the critical role of emission-wavelength modulation of CDs in the rational design of advanced PEC biosensors.
BACKGROUND: Most evidence on integrating primary eye care (PEC) into primary healthcare (PHC) comes from retrospective analyses of implementation successes or failures, often documenting challenges related to workforce skills, service compatibility, and health system constraints. However, far less attention has been given to assessing organizational readiness before implementation—despite readiness being a critical determinant of whether new service innovations can be effectively adopted and sustained. To address this gap, this study provides the first systematic, theory-informed evaluation of pre-implementation readiness for PEC–PHC integration, examining motivational, capacity-related, and contextual factors that may influence implementation success. METHODS: An explanatory sequential mixed-methods study was conducted in two rural counties in Xinjiang, China, during the pre-implementation phase of a stepped-wedge cluster randomized trial. Quantitative readiness data were collected using an adapted Organizational Readiness for Implementing Change (ORIC) tool, guided by the R = MC² heuristic. Participants included 14 township health center (THC) directors and 14 THC training doctors (selected via census), and 28 village doctors (selected via simple random sampling). For the qualitative phase, semi-structured interviews were conducted with 48 purposively sampled stakeholders. This included 42 providers derived from the quantitative sample, plus 6 county-level administrators and ophthalmologists. Quantitative data were analyzed using descriptive statistics, and qualitative data were analyzed using directed content analysis. Findings were integrated at the interpretation phase to explain quantitative scores through qualitative contextual insights, generating a comprehensive readiness profile. RESULTS: Overall readiness for PEC integration was moderate to high (mean composite score 3.63, SD 0.80). Motivation was the strongest dimension across cadres, with 85.7% of providers agreeing that PEC should be embedded within routine PHC services. Innovation-specific capacity showed greater variability, with THC training doctors demonstrating higher confidence in PEC skills than village doctors. General capacity exhibited the greatest constraints, including staffing shortages, limited equipment, and perceived workload burden. Qualitative findings revealed strong normative support for PEC integration but highlighted competing PHC priorities, uneven clinical skills, and structural resource limitations as key factors shaping readiness. Opportunities for integration were identified within existing public health programs and county medical alliance governance structures. CONCLUSION: This study underscores the critical value of assessing readiness before implementing new health service models. While rural providers in Xinjiang exhibit strong motivation to integrate PEC, disparities in capacity and persistent system-level constraints may hinder effective and sustainable implementation. The findings offer actionable insights for tailoring readiness-building strategies—including targeted training, supportive supervision, workflow integration, and policy alignment—to strengthen the feasibility of PEC–PHC integration and advance progress toward universal eye health coverage.
Previous studies have investigated the relationship between public environmental concern (PEC) and air pollution using annual-scale data. Due to the nonlinear and abrupt nature of public perception and response to sudden events, traditional methods may obscure the true causal relationship between PEC and air pollution. In this paper, we extend the measurement of PEC and use the Convergent Cross Mapping (CCM) to analyze its causal relationship with air pollution. Based on daily average PEC, AQI and PM2.5 data from January 1, 2023 to December 31, 2024 for 115 prefecture-level cities in China, we find that the relationship between PEC and air pollution exhibits nonlinear and weak coupling characteristics. At the same time, cities showing a significant causal effect of PEC on air pollution are predominantly situated in the North China Plain and the Yangtze River Economic Belt, regions characterized by relatively high levels of economic development. Compared to PEC affecting air pollution, air pollution significantly influences PEC in more cities. This result implies a reversed causal relationship in most cities, whereby air pollution is not alleviated by increased public environmental concern, but instead stimulates greater public attention to environmental issues through its adverse health impacts. PEC is effective as a pollution mitigation strategy only in a limited number of economically advanced cities. It is recommended that relevant departments introduce feasible policies that facilitate public feedback and reinforce the enforcement of environmental regulations and penalties. Relevant agencies should develop a more effective response framework, manage public attention data in a systematic and scientific manner, and explore region-specific approaches to utilize public environmental awareness to mitigate air pollution.
Here we present, for the first time, a light-encoded, dual-zone, single optical fiber (Zonal@OF)-based photoelectrochemical (PEC) microelectrode for the simultaneous and spatially resolved quantification of multiple biomarkers. To overcome the limitations of external light sources and rigid electrodes in conventional PEC biosensors, a single optical fiber was precisely etched to create two independent sensing zones (Zone I and Zone II). Each zone was sequentially functionalized with a gold nanoparticle conductive layer, a zone-specific light-harvesting material (BiOI nanoflakes for Zone I; methylene blue for Zone II), and a corresponding target-specific aptamer (for NT-proBNP and cTnI, respectively). The core innovation enables wavelength-resolved operation: upon separate excitation at 450 and 650 nm, the two zones generate distinct, noninterfering photoelectrochemical signals, allowing for the simultaneous, cross-talk-free detection of NT-proBNP and cTnI. The developed Zonal@OF-PEC sensor demonstrates high sensitivity at the pg mL-1 level, excellent specificity. By leveraging self-guided illumination and the miniaturized dimensions of optical fibers, along with achieving spatial-photonic encoding on a single fiber, this work demonstrates the potential of PEC biosensor to be further explored for real-time, multianalyte tracking. This capability bridges a critical gap toward their clinical translation in precision medicine.
Photoelectrocatalytic (PEC) technology integrates the advantages of both photocatalysis and electrocatalysis. It utilizes semiconductors to absorb sunlight as an energy source and applies a potential to facilitate the timely and directional transfer of photogenerated electrons, effectively achieving the physical separation of the photoanode and cathode. This is widely considered a primary factor in improving catalytic efficiency. In this study, In2S3 thin films and Au particles were prepared by hydrothermal and electrochemical deposition for robust attachment to TiO2 nanorods based on a fluorine-doped tin oxide (FTO) substrate, which greatly improves carrier transfer during the PEC process. The results showed that the cutoff wavelength of Au-In2S3/TiO2 was red-shifted to 535.6 nm. Under illumination without bias, the photoelectric current density of Au-In2S3/TiO2 reached 2.582 mA/cm2, 18-fold that of TiO2. Linear sweep voltammetry results indicated that under illumination at 0.8 V, the photoelectric current density of Au-In2S3/TiO2 was 7.956 mA/cm2, 24.7-fold that of TiO2, and 3.1-fold that of Au-In2S3/TiO2 under illumination without bias (0 V). The methanol-assisted test to amplify the hydrogen production signal revealed that, under illumination at 0.8 V bias (vs Ag/AgCl), the methanol-assisted hydrogen production rate of Au-In2S3/TiO2 was 2.51 mL/cm2, 3-fold higher than that under illumination alone (0.71 mL/cm2). This study provides new insights for methanol-assisted PEC hydrogen evolution reactions and serves as a reference for the design of high-performance photocatalysts.
The early and precise detection of cancer biomarkers is essential for effective cancer therapy. This study introduces a photoelectrochemical (PEC) biosensor specifically designed for the quantification of microRNA-106b (miR-106b), a biomarker linked to gastric cancer. The PEC biosensor was developed through the synthesis of tin(IV) oxide (SnO2) nanoparticles on the surface of fluorine-doped tin oxide (FTO) via a spin-coating method. Subsequently, an amino-modified single-stranded DNA (ssDNA) was immobilized onto the SnO2/FTO electrode, which was further modified with gold nanoparticles (AuNPs). The fabrication processes of the PEC biosensor were assessed by using electrochemical impedance spectroscopy (EIS) and PEC measurements. Upon hybridization of the probe attached to the biosensor with miR-106b, a substantial reduction in photocurrent was observed due to the obstruction of the electrode surface, resulting in the formation of a steric barrier. This steric hindrance limits the diffusion of ascorbic acid (AA) to the electrode surface, consequently decreasing the level of trapping of photogenerated holes. The photocurrent responses of the proposed biosensor exhibited linearity within a concentration range of 1.0 fM to 0.1 μM miR-106b, with a detection limit of 0.12 fM. The biosensor demonstrated the capability to detect miR-106b in sequences with a single base mismatch and noncomplementary bases. Furthermore, the biosensor was successfully employed to quantify miR-106b in human serum samples, yielding satisfactory results. The innovation of this research resides in the development of a photoelectrochemical biosensor specifically targeting miRNA-106b. The incorporation of electrodeposited gold nanoparticles on SnO2 spin-coated FTO represents an approach to enhancing the performance and sensitivity of the sensor. This biosensor has potential applications across a range of areas in the field of miRNA detection.
To identify actionable steps from a Veterans Health Administration (VA) Intensive Primary Care (IPC) pilot in five VA sites that primary care teams and health care systems can take to optimize medication regimens in high-risk patients, many of whom have polypharmacy and poor medication adherence. We conducted semi-structured, qualitative interviews between 2014 and 2018 with 27 IPC providers and 16 IPC patients. Interviews were analyzed using inductive and deductive approaches to thematic analysis. Patient respondents were an average of 67 years old and more likely to be male (94%), divorced (44%), Black (50%), hypertensive (88%), and have two or more comorbidities (81%). IPC patients and providers described IPC as helping to identify and/or address specific medication adherence barriers that were not adequately understood or addressed in usual primary care. IPC providers' greater understanding of adherence barriers allowed them to optimize patient medication regimens, closing the gap between care provided and patient needs. IPC program elements that enabled care improvements included interdisciplinary care teams, care team accessibility, home visits, and close provider-patient relationships. Primary care teams can adopt some IPC program elements to help patients optimize medication regimens, such as greater involvement of extended team members, increasing accessibility of care teams through telephone and secure messaging, utilizing home visits for assessment of patients' needs, and developing strong provider-patient relationships.
To investigate whether a questionnaire for Adolescent and Young Adults (AYAs), used to make an inventory of clinical care needs, can also be helpful to identify care needs of patients with early-onset colorectal cancer (eoCRC) (aged up to 50 years). To evaluate the content and usability of the questionnaire, semi-structured interviews with eoCRC patients treated with systemic therapy were conducted until data saturation was reached. Characteristics of respondents were reported. Interviews were transcribed verbatim, and analyses were performed using grounded theory. EoCRC patients perceived the questionnaire as a user-friendly tool to identify care needs. They long for more support on the themes family, support of children, interaction with family and friends and proactive care planning, depending on their phase of life and disease. Patients desire to discuss the questionnaire multiple times, because care needs change during the disease course. The questionnaire is a user-friendly tool to identify care needs of eoCRC patients. To improve care, patients emphasize that the questionnaire should be specified by phase of life and disease, include extra topics and offered several times. This study identifies unique care needs of patients with eoCRC and addresses topics to be improved in current care.
Learning health systems (LHS) use continuous data-driven learning cycles to improve care delivery, but seldom apply this approach to advance health equity. This perspective describes how the Veterans Health Administration (VA) applied LHS principles through a research-operations partnership between the Office of Health Equity (OHE) and the VA Health Equity-Quality Enhancement Research Initiative (QUERI) National Partnered Evaluation Center (PEC) to address racial and ethnic disparities in patient experience among VA users. The PEC analyzed the Survey of Healthcare Experience of Patients data to identify disparities in patient experience within VA regions (Veterans Integrated Service Networks [VISNs]). To address these disparities, OHE and PEC developed a "VISN equity toolkit" that communicates VISN-specific equity gaps by population group and patient experience metrics and offers tailored equity-guided quality improvement resources for distinct patient experience domains. For instance, in one VISN, Black veterans reported lower satisfaction with office staff helpfulness and respect versus White veterans, prompting focused strategies for staff training and service recovery programs. This research-operations partnership leverages LHS principles, aligns research and healthcare priorities, maps to existing frameworks for pursuing health equity through the LHS, and tailor interventions to regional needs to improve equity in VA patient care experience.
Integrating a hole transport layer (HTL) into photosensitive materials is a well-established strategy to bolster photoelectrochemical (PEC) performance, as it facilitates efficient charge carrier separation and directional migration. Herein, an innovative split-type PEC immunosensing platform based on ternary α-Fe2O3/CN/NiFe-layered double hydroxide (LDH) hierarchical architectures was strategically engineered. In this framework, nitrogen-doped carbon (CN) served as the HTL, establishing a high-efficiency charge extraction channel between the α-Fe2O3 core and the NiFe-LDH cocatalyst, which significantly suppressed non-radiative recombination. Following the specific immunorecognition of carcinoembryonic antigen (CEA), enzymatically generated H2O2 was introduced into the PEC cell as a potent hole scavenger to markedly augment the photocurrent signal. The resulting PEC immunosensor exhibited exceptional sensitivity and selectivity, with a wide linear range from 0.02 ng mL-1 to 50 ng mL-1 and a low detection limit of 7.21 pg mL-1. This work offers critical insights into the design of high-performance hole-transporting interfaces and the development of PEC sensing platforms for clinical diagnostics.
In this study, we report photoelectrochemical (PEC) detection technology for monitoring ClO- in natural water environments. This method demonstrates high sensitivity and selectivity, operational simplicity, and cost-effectiveness. To address the scarcity of existing PEC sensors for ClO-, a molecular hybridization strategy was employed to engineer a novel phenothiazine-chromone hybrid skeleton. By introducing a carboxyl group as an anchoring unit, we designed and synthesized a photoactive small molecule, CPTZ-COOH, which exhibits specific recognition toward ClO-. The carboxyl group enables effective immobilization of CPTZ-COOH onto a photoelectrode surface, serving as an organic photosensitizer. The resulting PEC platform, FTO/TiO2/CPTZ-COOH, exhibits a rapid, specific response to ClO- with a detection limit of 1.64 nM. Furthermore, the sensor demonstrates excellent performance in complex natural water matrices, offering a cost-effective and facile alternative for real-time environmental monitoring.
Solar-driven photoelectrochemical (PEC) production of chemical fuels such as hydrogen is a viable solution to address climate neutrality objectives. Development of a monolithic tandem PEC device consisting of ideal bandgap absorbers is of paramount importance to realize efficient artificial photosynthesis systems. Herein, we report monolithic integration of Sb2S3 on textured silicon to realize a completely inorganic and fully vacuum processed multilayer PEC device with Ag/Indium Tin Oxide (ITO)/Heterojunction with Intrinsic Thin layer (HIT) Si/ITO/Au/Sb2S3/NiOx architecture. Photoelectron spectroscopy and computational analysis show a staggered band alignment between Si and Sb2S3, emulating Z-scheme charge transfer mechanism. We demonstrate a high performing and stable Sb2S3-Si monolithic tandem for PEC hydrogen evolution reaction (HER) coupled to iodide oxidation reaction (IOR). Under AM 1.5G illumination, the Sb2S3-Si monolithic tandem device achieves unassisted photocurrent density of 4.38 mA cm- 2 with faradaic efficiency of 97% for hydrogen, while maintaining ∼90% of its initial performance after 10 h of continuous operation. These results set a new benchmark for all inorganic monolithic tandems for efficient and sustainable solar-to-chemical conversion. This work unlocks the pathway for artificial photosynthesis systems comprising ideal bandgap photo absorbers.
Photoelectrochemical (PEC) selective oxidation of glycerol offers a sustainable strategy to obtain dihydroxyacetone (DHA) as a value-added chemical, which remains challenging owing to the slow kinetics and low selectivity. We construct a Z-scheme heterojunction consisting of an amorphous vanadium oxide nanolayer on BiVO4 nanoparticles (BiVO4-VOx) for glycerol oxidation by a spatially confined photoelectron deposition method. BiVO4-VOx photoanode achieves a high DHA evolution rate of 400.4 mmol m-2 h-1 and a selectivity of 65.6% at 1.2 V vs. RHE. Femtosecond transient absorption spectroscopy analysis demonstrates superior charge separation efficiency and ultrafast interfacial transfer kinetics, enabling long-lived photogenerated electrons and holes accumulated in BiVO4 conduction band and VOx valence band, respectively. Furthermore, in situ Fourier transform infrared spectroscopy and theoretical calculations reveal that the synergy between the optimized electronic structure of amorphous VOx and Z-scheme heterojunction promotes preferential adsorption of glycerol middle hydroxyl groups and lowers the energy barrier of the rate-determining step, thus facilitating selective DHA production. We fabricated a self-powered device with a DHA productivity of 122.0 mmol m-2 h-1, a H2 productivity of 1.33 mL cm-2 h-1 and a solar-to-H2 conversion efficiency of 4.7%. This work highlights the potential of heterojunction engineering for PEC biomass valorization toward value-added products.
The Veterans Health Administration's (VHA) Community Care Network generally includes physicians with higher Medicare Merit-Based Incentive Payment System (MIPS) quality scores than nonparticipants, yet veterans disproportionately receive care from participating physicians with lower scores. Whether physician quality or availability influences veterans' use of community care has not been comprehensively evaluated. Our objective was to assess whether VHA community care specialists with higher MIPS quality scores receive greater referral volume or have longer wait times. We used multivariate regression models to assess the associations between physicians' MIPS quality scores, ranging from 0 to 100, and wait times or referral volumes. We also tested whether wait time moderated the association between physician quality and referral volume. We used administrative data to identify referrals to community-based specialists during 2021-2022. Referrals were then merged with MIPS quality scores from the Centers for Medicare & Medicaid Services using national provider identifiers. Our sample included 83,911 specialty care referrals involving 43,736 specialists. The mean MIPS quality score was 81.9 (SD = 20.9), including 77.9% of physicians who scored ≥ 75, the threshold for a positive payment adjustment. The overall mean wait time was 21.8 days (SD = 22.0), and the mean referral volume was 6.6 per year (SD = 10.5). In covariate-adjusted regression models, MIPS scores were not associated with wait times (+0.12 days per 10-point increase, 95% CI: -0.02, 0.25) or referral volumes (-0.15 referrals per 10-point increase, 95% CI: -0.37, 0.06). Wait time did not significantly moderate the relationship between MIPS score and referral volume. Physician quality appears to play a limited role in shaping referral decisions or access patterns in VHA community care. Although higher-scoring physicians sometimes have slightly longer wait times, these differences are small and do not translate into higher referral volumes.
Conventional antigen-antibody detection methods suffer from uneven antibody distribution and low target capture rates. Nevertheless, DNA offers an inherent advantage of structural tunability. By leveraging the DNA strand displacement reaction (SDR), DNA nanostructures can be ingeniously combined with photoelectrochemical (PEC) aptamer detection to effectively overcome the aforementioned limitations. Herein, an efficient "swing arm" DNA walker signal amplification strategy is designed to enhance PEC signal output. Introduction of AgInS2 quantum dots (AgInS2 QDs) into the sensing interface causes a marked decrease in the PEC signal. Upon entry of the carbohydrate antigen 15-3/aptamer (CA15-3/aptamer) complex into the sensing platform and subsequent release of the DNA probe modified with AgInS2 QDs (SP-AgInS2 QDs) from the interface, initial signal amplification is achieved. The system further employs exonuclease III (Exo III) enzymatic digestion to convert a "static" DNA tetrahedron (TDN) into a "swing arm" TDN, enabling multiple rounds of signal amplification. The resulting PEC aptamer sensor exhibits an excellent linear range (0.0001 - 200 U/mL) and a detection limit of 0.027 mU/mL. The designed strategy integrates "swing arm" TDN walkers with an aptamer sensor possessing high recognition capability. The strategy exploits the unique advantages of DNA nanostructures for signal cascade amplification and improved target capture rates. Furthermore, the sensing platform can be extended to other analytes by appropriately modifying the base sequences.
Photoelectrochemical (PEC) synthesis provides a sustainable route to produce adipic acid (AA) from cyclohexanone. However, the sluggish kinetics inherent to this complex multielectron-transfer process severely constrain the reaction efficiency. This paper describes a strategy to tune the oxidativity of surface-adsorbed hydroxyl species (*OH) for selective AA synthesis, implemented by integrating a Cu-doped cobalt hydroxide (Cu-Co(OH)2) cocatalyst onto a hematite-based photoanode. The as-prepared photoanode achieved an AA productivity of 10.4 μmol cm-2 h-1 with a Faradaic efficiency of 88.7% at 1.2 V vs RHE. Mechanistic study reveals that the incorporated Cu acts as an electronic modulator, inducing electron-deficient characteristics at the active Co sites. This electronic modulation effect enhances the electrophilicity of *OH, thereby boosting its intrinsic oxidative capacity. This study demonstrates a feasible pathway to tailor the oxidative capacity of active species via electronic modulation of the cocatalyst, providing new insights into the design of advanced PEC systems for the synthesis of value-added chemicals.
Pyro-photoelectrocatalytic (Pyro-PEC) water splitting integrates temperature fluctuations with solar irradiation to enable efficient hydrogen production, but conventional In2S3 suffers from weak photoresponse, rapid carrier recombination, and poor band alignment, limiting practical applications. To address these limitations, herein we first design and fabricate sulfur vacancy-mediated band bending and fermi level coupling VS-In1.90Y0.10S3 electrode, for synergistically enhance Pyro-PEC performance. Under Pyro-PEC conditions, the VS-In1.90Y0.10S3 electrode delivers a high current density of 2.79 mA cm-2 at 1.23 V vs. RHE, representing a 7.75-fold improvement over In2S3, along with significantly enhanced operational stability. Notably, we first employ in situ pyro-photoelectrochemical characterization to unveil that Y doped-induced sulfur vacancies can drastically amplify interfacial band bending and built-in electric field modulation under temperature fluctuations, thereby facilitating directed migration of photogenerated carriers and accelerating interfacial charge transfer. The performance enhancement originates from sulfur vacancy-mediated regulation of local defect states and band structure in In2S3, which elevates the Fermi level, optimizes carrier transport and energy distribution, and enables the synergistic reinforcement of Pyro-photoelectrocatalytic field effects under the combined stimuli of temperature fluctuation and photoexcitation. This work establishes a rare-earth doping-enabled defect engineering strategy, providing a novel material design paradigm and mechanistic insight for constructing high-performance Pyro-PEC hydrogen evolution electrodes.