CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yuanyuan Cong,Mengling Liu,Luyun Chen,Yurong Qi,Limin Zhang,Qiuping Zhao,Chunlei Li,Haibin Wang
The sluggish hydrogen energy conversion kinetics in alkaline medium and the complete passivation under high anodic potential as well as the easy detachment of active sites from the carbon substrate are three critical challenges of Ru-based electrocatalysts for their practical application. Herein, Ru (single atoms and nanoclusters)-embedded TiO 2-x (Ru SA -Ru NC /TiO 2-x ) well solves above-mentioned urgent problems simultaneously. Specifically, the optimal Ru SA -Ru NC /TiO 2-x electrocatalyst delivers a mass activity of 1620 A g Ru –1 and a low overpotential of 24 mV at 10 mA cm −2 in alkaline hydrogen oxidation and evolution reactions (HOR/HER), respectively. More importantly, the Ru/TiO 2-x can unprecedentedly catalyze the HOR up to a potential of 1.2 V vs. RHE without deactivation and almost maintain unchanged after accelerated stability tests of 10,000 CVs or the presence of 100 ppm CO impurity. Confirmed by in/ex-situ experimental measurements and computational analyses, the enhancement in performance is attributed mainly to the construction of high-density Ru-Ti bonds, maintaining the unblocked charge transfer from TiO 2 to Ru and achieving more low-valence Ru species. The observed Ti 3+ species on oxygen vacancies derived from the original structure and in-situ formation during the electrochemical reaction would be preferentially oxidized, further protecting Ru sites and aiding in the electrocatalytic process. Benefiting from Ru-Ti bonds and triggered oxygen vacancies, Ru could serve as exclusive optimal H adsorption sites and cooperate with the OH ad on Ti sites, rapidly and stably accelerating hydrogen energy conversion.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2018
·Vol. 20
·期 25
·17268-17278
·
IF 3.906
Weicheng Huang,Jinxin Wang,Lang Bian,Chaoyue Zhao,Danqing Liu,Chongshen Guo,Bin Yang,Wenwu Cao
A WO3−x/TiO2−x nanotube array (NTA) heterojunction photoanode was strategically designed to improve photoelectrocatalytic (PEC) performance by establishing a synergistic vacancy-induced self-doping effect and localized surface plasmon resonance (LSPR) effect of metalloid non-stoichiometric tungsten suboxide. The WO3−x/TiO2−x NTA heterojunction photoanode was synthesized through a successive process of anodic oxidation to form TiO2 nanotube arrays, magnetron sputtering to deposit metalloid WO3−x, and post-hydrogen reduction to engender oxygen vacancy in TiO2−x as well as crystallization. On the merits of such a synergistic effect, WO3−x/TiO2−x shows higher light-harvesting ability, stronger photocurrent response, and resultant improved photoelectrocatalytic performance than the contrast of WO3−x/TiO2, WO3/TiO2 and TiO2, confirming the importance of oxygen vacancies in improving PEC performance. Theoretical calculation based on density functional theory was applied to investigate the electronic structural features of samples and reveal how the oxygen vacancy determines the optical property. The carrier density tuning mechanism and charge transfer model were considered to be associated with the synergistic effect of self-doping and metalloid LSPR effect in the WO3−x/TiO2−x NTA.
研究领域:
材料科学
·
光催化
·
理论计算
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Lin Zhang,Xingda An,Kai Feng,Juan Li,Jingjing Liu,Jinxing Chen,Chaoran Li,Xiaohong Zhang,Le He
The interest in introducing light into heterogeneous catalysis is driven not only by the urgent need of replacing fossil energy but also by the promise of controlling product selectivity by light. The product selectivity differences observed in recent studies between light and dark reactions are often attributed to photochemical effects. Here, we report the discovery of a non-photochemical origin of selectivity difference, at essentially the same CO2 conversion rate, between photothermal and thermal CO2 hydrogenation reactions over a Ru/TiO2–x catalyst. While the presence of the photochemical effect from ultraviolet light is confirmed, it merely enhances the catalytic activity. Systematic investigation reveals that the gradual formation of an adsorbate-mediated strong metal–support interaction under catalytic conditions is responsible for the variation in the catalytic selectivity. We demonstrate that differences in product selectivity under light/dark reactions do not necessarily originate from photochemical effects. Our study refines the basis for determining photochemical effects and highlights the importance of excluding non-photochemical effects in mechanistic studies of light-controlled product selectivity.
研究领域:
催化
·
化学工程
·
物理化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Jiamin Li,Xiaoli Li,Guang Wu,Jiaqing Guo,Xiaohong Yin,Manman Mu
Visible light driven photocatalytic degradation of organic pollutants , such as bisphenol A (BPA) in wastewater, is considered as a promising strategy to solve the environmental issue . A two-dimensional (2D) porphyrin Co-TCPP MOF decorated 2D B-TiO 2−X nanosheet was successfully prepared through a facile hydrothermal method. The 2D–2D heterostructure could give rise to a built-in electric field to effectively promote the interfacial charge transfer and separation of photogenerated electron and holes. The presence of oxygen vacancy in the as-prepared heterostructure could greatly enhance the visible light harvesting ability to generate more photogenerated carriers. The Co-TCPP MOF@B-TiO 2−X exhibited remarkable photocatalytic performance for the degradation of BPA, whose degradation rate was up to 97% within 120 min irradiation. The degradation efficiency of this composite was 7.3 and 19.3 times higher than those of single Co-TCPP MOF and B-TiO 2−X respectively. The intimate contact between B-TiO 2−X and Co-TCPP MOF reduced interface resistance for charge migration, prolonged photoelectron lifetime and facilitated the charge carriers’ separation. The trapping tests verified that ·O 2 - was the mainly active species of BPA degradation. This strategy not only proves that the combination of B-TiO 2−X and Co-TCPP MOF is a feasible strategy to improve the photocatalytic degradation of BPA, but also provides some new inspirations for the construction of efficient 2D–2D composite photocatalysts.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jiaqing Liu,Jun Wan,Lin Liu,Weijie Yang,Jingxiang Low,Xiaoming Gao,Feng Fu
Aiming to the unwanted photocatalytic hydrogen production systems using sacrifice agents, a well-design S-scheme O-ZnIn 2 S 4 /TiO 2- x heterojunction was fabricated to realize photocatalytic hydrogen production via water reduction coupled with organic oxidative dehydrogenation. As supported by DFT calculations and experimental analysis, owing to the synergistic effect of oxygen defect and doping engineering, a tailored energy band structure alignment with higher redox potentials and larger Fermi level potential difference are achieved, resulting in more efficient S-scheme interface charge transfer and separation efficiency, thus improving the photocatalytic activity of O-ZnIn 2 S 4 /TiO 2- x . The optimal O-ZnIn 2 S 4 /TiO 2- x photocatalyst shows remarkable H 2 and benzaldehyde production rate of 2584.9 μmol g -1 h −1 and 2880.5 μmol g -1 h −1 under visible light, which are 52.5 and 66.4 times as high as those over blank TiO 2 . Interestingly, this coupled reaction system also displays superior H 2 evolution activity compared to sacrificial reagent systems of Na 2 SO 3 /Na 2 S and triethanolamine. Further quenching and EPR experiments reveal that both water and organic molecules provide protons for H 2 production.
研究领域:
材料科学
·
能源化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2026
·
IF 8.3
Dongxue Yu,Yimin Tang,Ziqi Liu,Lihui Hu,Xin Jiang,Bing Zhao,Libin Yang
Developing new-type semiconductor surface-enhanced Raman scattering (SERS) platform with synchronous enhancement of sensitivity and stability is an effective strategy for achieving ultra-sensitive detection of emerging pollutants in various pollution scenarios. In this work, a new g-C 3 N 4-x /N-doped TiO 2-x (g-C 3 N 4-x /N-TiO 2-x ) heterojunction SERS matrix was purposefully developed by a combined strategy of interface engineering and defect engineering. During the formation of heterojunction, “N-bidirectional migration” between two monomers can be achieved (that is, N vacancies and N doping can be generated simultaneously), which achieves a synchronous modulation of the atomic and electronic structures of the heterojunction. This endows g-C 3 N 4-x /N-TiO 2-x with excellent interfacial performance, abundant defect states, as well as ultra-high stability. The enhancement factor of the SERS matrix is as high as 10 9 . Theoretical calculations and experiments reveal the contribution of charge transfer (CT) mechanism to the SERS enhancement. The high-efficiency carrier separation induced by the strong interface coupling effect and the multi-channel CTs mediated by multiple defect states (vacancy defects and doping defects) are jointly responsible for the observed huge SERS enhancement. Benefiting from its high SERS sensitivity (selectivity) and excellent stability, g-C 3 N 4-x /N-TiO 2-x can be applied for ultrasensitive detection of antibiotic pollutants in multiple scenarios, including animal-derived foods such as milk, sour milk and beef, as well as natural water systems such as lake water and seawater. The detection limit of several typical antibiotic residues (enoxacin, ciprofloxacin, sulfamethoxazole and florfenicol) is as low as 1 × 10 −11 mol/L.
✓ 已验证
DOI
高影响因子
ACS Nano
·
2024
·
IF 15.8
Bo Chen,Wanmeng Wang,Meilin Hu,Yunkai Liang,Ning Wang,Changyi Li,Ying Li
The dental implant market has experienced explosive growth, owing to the widespread acceptance of implants as the core of oral rehabilitation. Clinically, achieving simultaneous anti-infective effects and rapid osseointegration is a crucial but challenging task for implants. The demand for implants with long-term broad-spectrum antibacterial and immune-osteogenic properties is growing. Existing methods are limited by a lack of safety, efficiency, short-lasting anti-infective ability, and inadequate consideration of the immunomodulatory effects on osteogenesis. Herein, a ZnO/black TiO2–x heterojunction surface structure was designed as a near-infrared (NIR) light-responsive nanofilm immobilized on a titanium (Ti) implant surface. This nanofilm introduces abundant oxygen vacancies and heterojunctions, which enhance the photothermal and photoelectric abilities of Ti implants under NIR illumination by narrowing the band gap and improving interfacial charge transfer. The “photo-thermo-electric” implant exhibits excellent broad-spectrum antibacterial efficacy against three dental pathogenic bacteria (Porphyromonas gingivalis, Fusobacterium nucleatum, and Staphylococcus aureus, >99.4%) by destroying the bacterial membrane and increasing the production of intracellular reactive oxygen species. Additionally, the implant can effectively eliminate mature multispecies biofilms and kill bacteria inside the biofilms under NIR irradiation. Meanwhile, this implant can also induce the pro-regenerative transformation of macrophages and promote osteoblast proliferation and differentiation. Moreover, in vivo results confirmed the superior antibacterial and osteoimmunomodulatory properties of this dental implant. RNA sequencing revealed that the underlying osteogenic mechanisms involve activation of the Wnt/β-catenin signaling pathway and bone development. Overall, this versatile “photo-thermo-electric” platform endows implants with anti-infection and bone integration performance simultaneously, which holds great potential for dental implants.
研究领域:
材料科学
·
生物材料
·
牙科材料
·
生物医学工程
·
免疫学
·
组织工程
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Acta Pharmaceutica Sinica B
·
2022
·
IF 14.903
Zekun Li,Yongchun Pan,Shiyu Du,Yayao Li,Chao Chen,Hongxiu Song,Yueyao Wu,Xiaowei Luan,Qin Xu,Xiaoxiang Guan,Yujun Song,Xin Han
Near-infrared (NIR)-light-triggered nanomedicine, including photodynamic therapy (PDT) and photothermal therapy (PTT), is growing an attractive approach for cancer therapy due to its high spatiotemporal controllability and minimal invasion, but the tumor eradication is limited by the intrinsic anti-stress response of tumor cells. Herein, we fabricate a tumor-microenvironment responsive CRISPR nanoplatform based on oxygen-deficient titania (TiO 2- x ) for mild NIR-phototherapy. In tumor microenvironment, the overexpressed hyaluronidase (HAase) and glutathione (GSH) can readily destroy hyaluronic acid (HA) and disulfide bond and releases the Cas9/sgRNA from TiO 2- x to target the stress alleviating regulators, i.e. , nuclear factor E2-related factor 2 (NRF2) and heat shock protein 90 α (HSP90 α ), thereby reducing the stress tolerance of tumor cells. Under subsequent NIR light illumination, the TiO 2- x demonstrates a higher anticancer effect both in vitro and in vivo . This strategy not only provides a promising modality to kills cancer cells in a minimal side-effects manner by interrupting anti-stress pathways but also proposes a general approach to achieve controllable gene editing in tumor region without unwanted genetic mutation in normal environments.
研究领域:
癌症治疗
·
纳米技术
·
基因编辑
·
光疗
·
生物材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）