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Nanoscale · 2022 ·Vol. 14 ·期 39 ·14520-14528 · IF 8.307

Interfacial Bi–S bonds modulate band alignment for efficient solar water oxidation

Weiwei Xu,Ningbo Fan,Shiji Xu,Linxing Meng,Bin Xu,Min Zhou,Wei Tian,Liang Li

Introducing suitable interfacial chemical bonds into heterojunctions can increase the charge carrier density, propel the charge separation, and facilitate interfacial charge extraction in photoanodes for photoelectrochemical (PEC) water oxidation. However, tuning chemical bonds at heterojunction interfaces and elucidating their influences on band alignment and the associated evolution of PEC performance remain elusive. Herein, Bi–S bonds were introduced into the interface of a CdIn2S4 (CIS)/Bi2WO6 (BWO) heterojunction. In situ irradiated X-ray photoelectron spectroscopy and electron spin resonance signals confirm that the Bi–S bond transforms the band alignment from type II to the direct Z-scheme, significantly enhancing the carrier separation efficiency. Theoretical calculations show that the Bi–S bond not only acts as an atomic-level charge transfer channel, but also changes the migration pathway and distance within the heterojunction. As a result, the optimized CIS/BWO photoanode exhibits a relatively high PEC performance of 4.25 mA cm−2 at 1.23 V vs. RHE (VRHE) and a low onset potential of 0.30 VRHE. This work presents a new avenue to construct comprehensively improved photoanodes by tuning the interfacial structures at the atomic level.

研究领域: 材料科学 · 光化学 · 电化学 · 可再生能源
✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

A visible and near-infrared light dual-responsive PEC immunosensor for archaeological silk microtrace detection based on in situ growth of Ag2S on ZnO-MXene nanocomposites

Qingqing Zhou,Yong Liu,Lin Wang,Kun Wang,Haodong Chen,Hailing Zheng,Yang Zhou,Zhiwen Hu,Zhiqin Peng,Junmin Wan,Bing Wang

Developing an effective analytical method for microtrace detection of ancient silk is highly desirable and vitally crucial for exploring the origin and spread of silk. Herein, a taxonomically specific anti-fibroin monoclonal antibody was prepared and an elaborate visible/near-infrared (vis/NIR) photoelectrochemical (PEC) immunosensor was proposed. The sensor employed Ag 2 S nanoparticles (NPs) grown in situ on ZnO nanowire array-MXene nanocomposites (ZnO-MX) via a sonochemical method as a photosensitive material. The experimental results illustrated that the ZnO-MX/Ag 2 S-based sensor presented 6.8 times larger PEC responses than a ZnO-MX-based sensor under visible light illumination, and the PEC signal of the ZnO-MX/Ag 2 S nanocomposites was 30 times as high as that of ZnO-MX under 808 nm NIR light, indicating enhanced photoelectric activity and a matched energy band structure of ZnO with MXene and Ag 2 S. This PEC immunosensor exhibited excellent potential for the ultrasensitive detection of Bombyx mori silk traces due to its wide linear range of 0.005–50 ng mL −1 and low detection limit of 1.51 pg mL −1 . Additionally, the immunosensor showed outstanding specificity, stability, and repeatability, particularly for the qualitative detection of archeological artifacts. Given its aforementioned benefits, ZnO-MX/Ag 2 S nanocomposites are potentially attractive photoactive materials for use in vis/NIR PEC immunosensors. Moreover, this demonstrated method offers a feasible method to investigate the history and distribution of ancient silk.

研究领域: 考古学 · 生物传感 · 材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

A cobalt silicate modified BiVO4 photoanode for efficient solar water oxidation

Qi Sun,Ting Cheng,Zhirong Liu,Limin Qi

BiVO 4 is one of the most promising photoanode materials for photoelectrochemical (PEC) water splitting, but it usually suffers from severe charge recombination. In this work, cobalt silicate (Co-Sil) was decorated on a nanoporous BiVO 4 photoanode as a novel cocatalyst by photoelectrophoretic deposition that integrated photoelectrochemical oxidation and electrophoretic deposition. The resultant BiVO 4 /Co-Sil photoanode reached a photocurrent density of 5.0 mA/cm 2 at 1.23 V RHE , around 3-fold enhancement compared with the pristine BiVO 4 photoanode. Detailed PEC measurements combined with density functional theory calculations revealed that the excellent performance of the Co-Sil cocatalyst could be attributed to the electron transfer from Co-Sil to BiVO 4 , the reduced overpotential of the OOH* formation, and the photoelectrochemical oxidation of Co(II). Furthermore, a high photostability was achieved for the BiVO 4 /Co-Sil photoanode by dissolving NaVO 3 in the electrolyte. This work may provide new insights on the rational design and effective fabrication of promising cocatalysts for solar water splitting.

研究领域: 材料科学 · 光化学 · 电化学 · 可再生能源
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BIOSENSORS & BIOELECTRONICS · 2015 · IF 6.409

A label-free photoelectrochemical aptasensor based on nitrogen-doped graphene quantum dots for chloramphenicol determination

Yong Liu,Kai Yan,Otieno Kevin Okoth,Jingdong Zhang

A photoelectrochemical (PEC) sensing platform for chloramphenicol (CAP) detection was constructed using nitrogen-doped graphene quantum dots (N-GQDs) as transducer species and label-free aptamer as biological recognition element . N-GQDs, synthesized via a facile one-step hydrothermal method , were explored to achieve highly efficient photon-to-electricity conversion under visible light irradiation . The obtained N-GQDs were characterized by transmission electron microscopy (TEM), which displayed a narrow size distribution with a mean diameter of 2.14   nm. The X-ray photoelectron spectroscopic (XPS) and Fourier transform infrared spectroscopic (FT-IR) analysis confirmed that nitrogen was successfully doped in GQDs. The UV–visible absorption spectra indicated that nitrogen doping obviously enhanced the absorption of GQDs in visible light region. As a result, the PEC activity of GQDs was promoted by nitrogen doping. Additionally, the π-conjugated structure of N-GQDs provided an excellent platform for aptamer immobilization via π–π stacking interaction. Such an aptamer/N-GQDs based sensor showed a linear PEC response to CAP concentration in the range of 10–250   nM with a detection limit (3 S/N) of 3.1   nM. The developed PEC aptasensor exhibited high sensitivity and selectivity , good reproducibility and high stability.

研究领域: 分析化学 · 环境科学 · 生物传感器 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2019 · IF 6.361

Preparation of P-g-C3N4-WS2 nanocomposite and its application in photoelectrochemical detection of 5-formylcytosine

Fei Li,Huanshun Yin,Yan Chen,Siyu Wang,Jingyan Li,Yuemei Zhang,Chunxiao Li,Shiyun Ai

DNA formylation (5-formylcytosine, 5fC) is a major epigenetic modification involved in alterations in the DNA double helix structure and protein identification. Due to the low amount in all mammalian tissues and cells, it is necessary to develop a rapid, sensitive and efficient method for detecting 5fC for further understanding the biological functions of 5fC. Thus, a novel PEC biosensor was constructed using P-g-C 3 N 4 -WS 2 nanocomposite as photoactive material. Firstly, AuNPs/P-g-C 3 N 4 -WS 2 /ITO electrode was prepared as substrate electrode. Secondly, the probe DNA and complementary DNA (containing 5fC base) was modified to the electrode surface based on the formation of Au-S bonds between AuNPs and thiol group on the probe DNA and hybridization, respectively. Finally, the amino functionalized MnO 2 nanoflowers were further modified to the electrode surface by covalent interaction between the aldehyde group on the 5fC and the amino group on MnO 2 nanoflowers. The sensitive and specific detection of 5fC can be achieved by oxidizing ascorbic acid with MnO 2 nanoflowers and quenching the photoactivity of P-g-C 3 N 4 -WS 2 nanocomposite. The sensor has a detection range of 0.01–200 nM and a detection limit of 3.8 pM. Moreover, this sensor has excellent detection specificity, stability and reproducibility.

研究领域: 生物化学 · 分析化学 · 表观遗传学 · 纳米技术
✓ 已验证 DOI PubMed 高影响因子
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BIOSENSORS & BIOELECTRONICS · 2019 · IF 9.518

Dual-readout immunosensor constructed based on brilliant photoelectrochemical and photothermal effect of polymer dots for sensitive detection of sialic acid

Jiani Wang,Shupei Zhang,Hong Dai,Hongli Zheng,Zhensheng Hong,Yanyu Lin

A delicate dual-readout immunosensor based on tetraphenylporphyrin-polymer dots (TPP-Pdots) with brilliant photoelectrochemical and photothermal performance was first successfully fabricated for the ultrasensitive detection of sialic acid (SA). Herein, TPP-Pdots with good biocompatibility , extraordinary light-harvesting ability and excellent photothermal conversion efficiency was used to capture SA antibody as dual-functional bioprobe for generating photocurrent and temperature signal. Furthermore, the large surface and morphology-mediated of rutile-TiO 2 (R–TiO 2 ) was beneficial to load amounts of TPP-Pdots for improved PEC signal and photothermal signal. Importantly, the temperature readout resulted from the variation of target concentration could be easily obtained by a universal thermometer which was time-saving and cost-saving. Under the optimized experimental conditions, the photocurrent densities and temperature changes proportionally increased with the increasing of SA concentrations from 3.5 × 10 −5  ng/mL to 35 ng/mL (R = 0.996). Impressively, the dual-readout approach proposed here not only featured with good accuracy and high sensitivity for SA detection, but also paved the way for the development of a dual-readout immunoassay based on PEC biosensor.

研究领域: 分析化学 · 生物传感器 · 纳米技术 · 生物医学工程
✓ 已验证 产品关联 DOI PubMed 高影响因子
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BIOSENSORS & BIOELECTRONICS · 2017 · IF 7.78

A sensitive photoelectrochemical immunoassay of N6-methyladenosine based on dual-signal amplification strategy: Ru doped in SiO2 nanosphere and carboxylated g-C3N4

Haiyan Wang,Chunling Qi,Wenhuan He,Minghui Wang,Wenjing Jiang,Huanshun Yin,Shiyun Ai

A novel, simple and sensitive photoelectrochemical (PEC) immunosensing platform was constructed for detecting N 6 -methyladenosine (m 6 A) based on the carboxylated CN and avidin functionalized [email protected] 2 (ARS) nanocomposite . Herein, the N 6 -methyladenosine-5′-triphosphate (m 6 ATP) was selected as the detection target molecule, m 6 A antibody was used as recognition unit for m 6 A, the carboxylated g-C 3 N 4 (CN) was not only used as the photoactive substance, but the substrate for the m 6 A antibody immobilization , ARS was synthesized and used as signal amplification unit to improve the photocurrent of CN, Phos-tag-biotin was employed as bridge of m 6 ATP and [email protected] 2 through the specific interaction between phosphate group of m 6 ATP and Phos-tag, biotin and avidin, respectively. Under the optimal condition, the fabricated PEC biosensor showed a linear range of 0.01–10   nM and high detection sensitivity with low detection limit of 3.23   pM for m 6 ATP. Besides, the developed strategy was also successfully applied to evaluate the content of m 6 A in human serum samples.

CAS / MDL: 50-81-7 60-00-4 77-86-1
研究领域: 分析化学 · 生物化学 · 纳米技术 · 生物传感器
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

A novel photoelectrochemical system to disrupt microalgae for maximizing lipid-extraction efficiency

Yongwu Wu,Wenhao Xiang,Linyang Li,Huimin Liu,Nianbing Zhong,Haixing Chang,Bruce E. Rittmann

Microalgae biodiesel is a candidate to provide renewable, C-neutral energy. However, microalgal cells possess strong cell walls and cell membranes with high selective permeability, both of which hinder the extraction of lipids from the microalgae. Optimizing lipid extraction involves disrupting the microalgae’s cell wall and membrane. The hydroxyl free radical ( • OH) can attack the cell wall and cell membrane in the microalgae, making the microalgae more susceptible to lipid extraction. Introduced here is a PhotoElectroChemical (PEC) with TiO 2 -based photoanode utilized UV–Vis light to produce • OH at a phosphate-palladium cathode. Until now, PEC has not been utilized to disrupt microalgal cells to improve the extraction of microalgae lipids. Here, a novel PEC system -- comprised of two nitrogen-doped TiO 2 nanotube photoanodes, a bipolar membrane, and a phosphorus-palladium cathode -- was demonstrated to disrupt microalgal biomass to improve lipid extraction. PEC utilizes ultraviolet and visible light as the only input energy for the effective disruption of the microalgal cell. Pretreatment of Chlorella using the PEC system resulted in 96% oil-extraction efficiency which was approximately 10 times higher than that achieved without the pretreatment and an increases in desirable C16:0. Also explored were the mechanisms underlying • OH generation and microalgae disruption. PEC promises to be an eco-friendly and low-energy technology that can promote the development of microalgae industries.

研究领域: 生物工程 · 可再生能源 · 环境科学 · 生物技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Solar-powered enzymatic-photoelectrocatalytic system constructed with three-dimensional dual photoelectrodes for highly efficient purification of coking wastewater

Jianqiao Liu,Jinli Wang,Jiang Guo,Kai Yan,Jingdong Zhang

The coupling of photoelectrocatalysis (PEC) and enzymatic catalysis was explored for efficient treatment of practical phenol-containing coking wastewater outdoors. The developed enzymatic-photoelectrocatalytic (EPEC) system consisted of three-dimensional dual photoelectrodes fabricated with carbon fiber cloth (CFC), namely a CFC-supported WO 3 photoanode with oxygen vacancies and a CFC-supported Au-BiOBr photocathode with immobilized horseradish peroxidase (HRP). The experimental results and computational fluid dynamics study revealed that dual CFC-based photoelectrodes with three-dimensional network structures could optimize the fluid diffusion on the electrode surface and enhance the efficiency of pollutant degradation. Further investigation indicated that the introduction of oxygen vacancies promoted the PEC oxidation activity of the WO 3 photoanode while the Au nanoparticles modification was favorable to improving the immobilization of HRP and PEC generation of H 2 O 2 on BiOBr photocathode. Moreover, photovoltaic (PV) cells were integrated in the EPEC system to provide applied potential and promote the utilization of solar irradiation. The mineralization rate of coking wastewater reached 88.5% using the PV-integrated EPEC system driven by natural solar energy, which demonstrated potential for treating actual industrial wastewater.

研究领域: 环境科学 · 电化学 · 废水处理 · 可再生能源 · 催化
✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

A BiVO4 film photoanode with re-annealing treatment and 2D thin Ti3C2TX flakes decoration for enhanced photoelectrochemical water oxidation

Dejian Yan,Xingchen Fu,Zhichao Shang,Jikai Liu,He'an Luo

Bismuth vanadate (BiVO 4 ) has been envisioned as a promising photoanode material for photoelectrochemical (PEC) water oxidation. However, the PEC performance of BiVO 4 based photoanodes is usually dragged down by the poor charge transport and slow kinetics for an oxygen evolution reaction (OER). Here, a novel composite photoanode of Ti 3 C 2 T X /BiVO 4 was fabricated for the first time by spin coating thin Ti 3 C 2 T X (MXene) flakes onto the surface of a BiVO 4 film grown on the FTO substrate. A facile re-annealing treatment of bare BiVO 4 /FTO photoanode in argon can impressively boost the photocurrent density from 2.1 mA cm −2 up to 2.95 mA cm −2 . Experimentally, we clearly elucidated that by re-annealing, the interfacial (BiVO 4 /FTO) charge recombination could be effectively suppressed due to the better contact between the BiVO 4 film and FTO. The coating of thin Ti 3 C 2 T X flakes onto the BiVO 4 film would further increase the photocurrent density to 3.45 mA cm −2 (measured at 1.23 V vs. reversible hydrogen electrode (RHE) under 1 sun illumination), exhibiting a photoconversion efficiency of 0.78% and a surface charge separation efficiency of 73%. The outstanding PEC performance can be mainly ascribed to the coating of the thin Ti 3 C 2 T X (MXene) flakes which function as co-catalysts, facilitating the charge transfer of the photogenerated carriers and reducing the charge recombination on the BiVO 4 surface. Our findings provide a facile re-annealing strategy and a novel two-dimensional (2D) material of Ti 3 C 2 T X (MXene) as co-catalysts to improve the performance of the BiVO 4 photoanode for PEC water oxidation.

研究领域: 材料科学 · 电化学 · 可再生能源 · 纳米技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Accelerating charge separation in p-n heterojunction photocathode for photoelectrochemical oxygen reduction and evolution in photo-enhanced zinc-air battery

Yunong Qin,Chengrun Liu,Xin Peng,Zhixin Ma,Ling Li,Song Chen,Wenming Zhang

For the first time, we constructed a band-matched ZnO/NiO staggered p-n heterojunction photoelectrochemical (PEC) catalyst with superior charge separation and transfer efficiency to optimize the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) kinetics demands of a photo-enhanced zinc-air battery (PZAB). The ingenious design of heterojunction architecture effectively stimulates an internal self-built electric field (BEF), thus accelerating charge separation and migration during PEC catalysis. Upon illumination, the photocathode not only endows a promoted PEC catalytic competence to drive ORR and OER, but also reduces the charge–discharge voltage gap of PZAB. Density functional theory (DFT) calculations further disentangled the PEC catalysis activity origins by substantiating the strongly decreased Gibbs free energy potently for generating the essential intermediates *OH and *OOH during ORR and OER, respectively, and visualized the charge densities in photocathode to illustrate the authentic separation of photogenerated carriers. Remarkably, our work experimentally and theoretically sheds lights on engineering innovative and efficient bifunctional PEC catalysts to drive PZABs with photo-enhancement.

研究领域: 材料科学 · 电化学 · 催化 · 能源存储与转换
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RSC Advances · 2019 ·Vol. 9 ·期 72 ·42533-42542 · IF 3.049

A carbon-rich nanofiber framework based on a conjugated arylacetylene polymer for photocathodic enzymatic bioanalysis

Junyan Tang,Xiaoya Liu,Chengwei Yang,Zhening Zhang,Rui Sun,Hongmei Li,Caolong Li,Fei Wang

Poly(1,3,5-triethynylbenzene) (PTEB), a newly developed conjugated arylacetylene polymer, was utilized for photoelectrochemical (PEC) enzymatic bioanalysis in this work. The porous nanofiber framework of PTEB film which produced an apparent cathodic photocurrent under visible light illumination was fabricated on an indium tin oxide (ITO) electrode via copper-surface mediated interface Glaser polycondensation. As the photocurrent density of the metal-free photocathode displayed a characteristic O2 dependency, the consumption of dissolved oxygen caused by the modified glucose oxidase (GOx) in biocatalysis induced a depressed photoresponse in the presence of glucose. The fabricated PEC transducer exhibited favorable glucose sensing performances in the linear range of 5 μM to 8 mM and with the detection limit of 1.7 μM; it could also be employed in glucose monitoring in human serum. Moreover, the acetylenic carbon-rich polymer possessed the superior features of being cost-effective in preparation and machinable in device development, which sheds light on the exploration of an advanced PEC sensing platform based on conjugated organic polymers for the bioanalysis of valuable analytes.

研究领域: 材料科学 · 生物化学 · 分析化学 · 纳米技术
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