Inorganic Chemistry Frontiers
·
2026
·
IF 6.2
Chaofan Deng,Chun Cai
Achieving direct cleavage of CO bonds in biomass under mild conditions to generate high-value-added products via catalytic hydrogenation remains a substantial challenge. We developed a Pd–Fe bimetallic catalyst supported on oxygen vacancy (Ov)-enriched TiO2 for the direct cleavage of CO bonds, and as a result, up to 99% yield of 2-methoxy-4-methylphenol (MMP) was achieved from the conversion of vanillin (VAN) at 140 °C under atmospheric H2 pressure. This study utilizes Ov to enhance hydrogen spillover levels during the reaction process and proposes a novel reaction pathway that avoids the formation of alcohol intermediates. Mechanistic investigations reveal that surface Ov facilitates hydrogen spillover, enabling active hydrogen migration from Pd–Fe sites to TiO2 to form Ti–H species. Through synergistic Pd–Fe bimetallic effects and metal–support interfacial interactions, direct hydrodeoxygenation (HDO) of VAN is achieved, ultimately generating MMP with high selectivity. The catalyst demonstrates excellent stability and broad substrate suitability, maintaining uncompromised activity after five catalytic cycles.
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ACS Catalysis
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2020
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IF 12.35
Zean Xie,Tingting Yu,Weiyu Song,Jianmei Li,Zhen Zhao,Baijun Liu,Zhenfei Gao,Dong Li
The research and development of abundant, non-toxic, low cost, and high-performance catalysts are urgently required for the production of propylene through propane dehydrogenation (PDH) reaction. Here, the pure TiO2 nanoparticles, obtained through in situ reduction, exhibit excellent catalytic PDH performance. At 600 °C, the initial propane conversion could reach 67%, and the one-pass yield of propylene was 45%. The propane conversion was 21% at 550 °C, and propene selectivity could reach as high as 94%. According to ex/in situ characterization results and Quantum chemical calculations, the dynamic formation and reaction mechanism of active sites were detailedly investigated. The reductive propane and its derivatives can react with surface lattice oxygen of nanosized anatase TiO2 to form oxygen vacancies and coordinatively unsaturated Ti cations (Ticus), which can catalyze PDH with high propene selectivity; the rate of C3H6 formation is in line with the surface oxygen vacancy concentration. Notably, the Ostwald ripening of nanosized TiO2 with high surface energy is crucial to the formation of oxygen vacancies. The agglomeration of nanosized TiO2 at high temperature makes the lattice oxygen atoms mobile and active, which are consumed abruptly and then form oxygen vacancies and Ticus more easily. It is denoted as “mutation reduction”. The surface oxygen vacancy concentration is also influenced by the oxygen migration rate from bulk to surface driven by thermal energy and potential energy (the differences of concentration).
研究领域:
催化化学
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材料科学
·
量子化学
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Journal of Physical Chemistry C
·
2018
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IF 4.484
Chengzhang Zhu,Xiao Chen,Jian Ma,Cheng Gu,Qiming Xian,Tingting Gong,Cheng Sun
Inducing TiO2 sensitive to visible light and effectively restraining the possibility of electron–hole recombination are crucial for actual applications over TiO2-based catalysts. In this study, a facile strategy to fabricate three-dimensional (3D) defective TiO2–x@carbon spheres (CSs) composite modified with two-dimensional (2D) graphite-like carbon nitride (g-C3N4) nanosheets (NSs) is presented. During the synthesis process, zero-dimensional tiny TiO2–x nanoparticles were evenly loaded onto CSs with intimate chemically bonded (Ti–O–C) interfaces. Simultaneously, loose g-C3N4 NSs were tightly coated on the hierarchical spherelike TiO2–x@CSs, with the purpose of supporting an effectively protective layer to prevent the oxidation of the directly exposed Ti3+ and constructing highly efficient 2D/3D ternary heterostructures with strong interfacial interaction. The obtained CSs/TiO2–x@g-C3N4 heterojunction showed remarkably enhanced photocatalytic activity in hydrogen production and toxic pollutants degradation compared to the binary composites or pristine components, mainly due to the cooperative effects of the enhanced visible-light-harvesting capacity introduced by Ti3+ and CSs, effective interfacial charge separation (Ti–O–C structure and heterostructure), and the vectorial charge-transfer channel design. This work paves a green, gentle, and economical way to design more efficient TiO2–x new ternary materials with multistep electron transfer toward solar energy conversion (like CO2 reduction and H2 evolution).
研究领域:
材料科学
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环境科学
·
化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Ben Chen,Jin Zhang,Jing Yu,Rui wang,Beibei He,Jun Jin,Huanwen Wang,Yansheng Gong
Poor visible light utilization and charge separation efficiency of TiO 2 restrict its extensive application in the photocatalytic field. Herein, a specific Z-scheme TiO 2-x /Cu/ZnO heterojunction was successfully constructed by atomic layer deposition (ALD) technique and spray pyrolysis technology. Benefited from the surface plasmon resonance (SPR) effect of Cu and Z-scheme heterojunction, the visible light absorption capacity was greatly enhanced. Meanwhile, ZnO nanolayer coating, prepared by ALD technique, protects Cu element to hinder its oxidation, thus enhancing the separation efficiency of photogenerated carriers. Therefore, the photocatalytic hydrogen production performance was significant improved, exhibiting a maximum value of 342.0 µmol·g −1 ·h −1 for the optimal B-T-0.1C-10Z (black TiO 2 /0.1Cu/10 nm ZnO) sample without any noble-metal cocatalyst, which is higher than pure TiO 2 (310.7 µmol·g −1 ·h −1 , with 3 wt% Pt) synthesized by spray pyrolysis method under equal conditions. In addition, a possible mechanism for the enhanced performance was briefly discussed based on the experimental results.
研究领域:
材料科学
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光催化技术
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表面化学
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PubMed
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Energy & Environmental Materials
·
2026
·
IF 14.1
Bingke Zhang,Chenchen Zhao,Jing Qiao,Changcun Li,Yang Wang,Xingshuo Liu,Dongbo Wang,Gang Liu,Zhao Qian,Rajeev Ahuja,Jinzhong Wang,Degang Zhao
Solar-driven photothermal CO 2 reduction into multicarbon (C 2 + ) products represents a promising yet challenging route for sustainable fuel production. A key obstacle remains the inefficient C–C coupling due to poor CO 2 activation and limited charge utilization, especially under full-spectrum light. Herein, we propose a heterojunction photocatalyst that synergistically integrates the topological insulator Bi 2 Te 3 with oxygen-doped TiO 2-X to address these challenges. The metallic nature of Bi 2 Te 3 enables broad-spectrum photon harvesting from UV to near-infrared and generates substantial photothermal heat, while the oxygen vacancies in TiO 2-X create an asymmetric electronic environment that promotes CO 2 adsorption, bending, and activation. The built-in electric field formed at the heterointerface drives efficient electron transfer from Bi 2 Te 3 to TiO 2-X , which suppresses charge recombination and ensures a prolonged electron supply for multistep reduction reactions. Under full-spectrum irradiation without external heating, the optimized Bi 2 Te 3 /TiO 2-X catalyst achieves a remarkable C 2 + production rate of 15.08 μmol g −1 h −1 with selectivity toward C 2 H 4 and C 2 H 6 . Combined photoelectronic measurements and theoretical analyses confirm that the synergistic photothermal–photocatalytic effect and tailored charge dynamics collectively lower the energy barrier for C–C coupling. This work offers a strategic material design leveraging topological insulators and defect engineering for efficient CO 2 -to-C 2 + conversion.
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2026
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IF 5.9
Qian Tang,Wen-Li Luo,An-Ni Guo,Yuan Chen,Zhen-Hua Liu,Jing-Wei Shao
Nanozyme heterostructures with extended light absorption into the visible region. • Chlorogenic acid-loaded microneedles enable bidirectional ROS regulation. • Dynamic redox homeostasis promotes M2 polarization and angiogenesis. • The microneedle platform enables synergistic antibacterial and wound-healing therapy. Burn wounds infected with Staphylococcus aureus (S. aureus) are often characterized by excessive early inflammation, which leads to persistent oxidative stress, pain, and delayed healing. To overcome the limitations of conventional photosensitizers, which may induce reactive oxygen species (ROS) overload and subsequent tissue damage, we developed a ROS-responsive microneedle patch (TC@MN). This system consists of chlorogenic acid–based microneedles encapsulating a CuₓO–TiO 2-X (TC) nanozyme heterostructure designed for synergistic antibacterial and regenerative therapy. TC@MN exhibits intrinsic peroxidase-like (POD) and catalase-like activities (CAT). Under light irradiation, these catalytic processes participate in ROS regulation and promote Cu²⁺/Cu⁺ redox cycling, leading to the generation of bactericidal •OH and •O₂⁻ radicals while simultaneously producing O₂ to alleviate local hypoxia. In animal experiments, TC@MN scavenges excess ROS and promotes macrophage polarization toward the M2 phenotype thereby facilitating inflammation resolution and tissue repair under light-free conditions. Collectively, this light/dark dual-mode microneedle platform integrates photocatalytic and enzyme-mimetic functions, offering a biocompatible and intelligent strategy for the treatment of infected burn wounds.
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高影响因子
APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Hongli Fang,Yuanqing Kang,Shaotang Yuan,Miaomiao Zhang,Zebao Rui
Titanium dioxide (TiO 2 ) is a widely used low-cost and stable photocatalyst, but its wide bandgap and low quantum efficiency usually lead to poor photocatalytic performance. Herein, one-step solid state calcination and reduction method was proposed for simultaneously introducing surface defects and loading Ag nanoparticles (NP) on TiO 2 . The as-obtained black TiO 2-x supported Ag NP (or Ag/TiO 2-x ) holds a narrow bandgap to respond to the full solar spectrum due to the presence of high concentration surface vacancies, enhanced light absorption through the surface plasmon resonance effect of Ag NP, and satisfactory photothermal effects. Moreover, such a one-step solid state synthesis method leads to closely linked interface and enhanced charges transfer between Ag NP and TiO 2-x . Accordingly, Ag/TiO 2-x exhibits robust photothermal synergistic VOCs degradation performance with a toluene degradation rate 6 times higher than the reference Ag/TiO 2 (DP) prepared by the conventional solution method.
研究领域:
材料科学
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环境科学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2026
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IF 4.6
Guofa Sun,Ziwei Pan,Man Zhang,Shaozhi Yang,Peng Yang,Jincheng Chen,Xie Fu,Wenqiang Lu
Lithium‑sulfur (Li-S) batteries are a highly promising energy storage technology due to their exceptionally high theoretical energy density. However, their practical implementation faces significant challenges, including sluggish redox kinetics and the troublesome shuttling of lithium polysulfides (LiPSs). In this work, a hierarchical TiO 2-x nanostructure was utilized as the sulfur host. Sulfur was uniformly integrated into the structure through a melt-diffusion infiltration process. The introduced oxygen vacancies in TiO 2-x provide strong chemical adsorption of polysulfides, effectively suppressing the shuttle effect and reducing active material loss. The nanoflower architecture-composed of interconnected nanosheets-offers a high specific surface area (104.45 m 2 g −1 ) and large pore volume (0.4698 cm 3 g −1 ). This design not only increases the number of accessible active sites but also helps accommodate volume changes during cycling. Furthermore, electron paramagnetic resonance (EPR) confirms the abundance of oxygen vacancies, which act as catalytic sites to enhance polysulfide anchoring and accelerate Li 2 S nucleation kinetics. As a result, the TiO 2-x -CNS@S cathode achieves a high initial discharge capacity of 1398 mAh g −1 at 0.1C and demonstrates remarkable long-term cycling stability. At 1C, it maintains an ultralow capacity decay rate of 0.054% per cycle over 1000 cycles. This dual-functional host design offers an effective and scalable strategy to simultaneously improve reaction kinetics and cycling durability in high-performance Li-S batteries.
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Nanomaterials
·
2025
·Vol. 15
·期 7
·514
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IF 4.3
Man Zhou,Yanli Zhou,Minmin Ni,Yuzhe Zhang,Song Xu,Hao Ma,Jian Zhou,Jin Zhao,Liwei Lin,Zhongyu Li
Superior selective adsorption of organic dye is still a big challenge in the process of dye wastewater treatment. Meanwhile, low-price and environmentally friendly biomass-based adsorbents show huge potential in the fields of separation and purification. In this study, we adopted the “hydrolysis–calcination method” to develop a novel in situ anchoring strategy for ultrasmall TiO2−xon carbonized bacterial cellulose (CBC), which was derived from natural bacterial cellulose. Notably, 3D networks of porous CBC played a dual role for both providing hydrolytic sites and controlling the oxygen vacancies (Vo) of TiO2−x. As for the single-dye adsorption, the TiO2−x/CBC had a strong adsorption ability (101.4 mg/g) for removing methylene blue (MB), which was much higher than that of methyl orange (MO), malachite green (MG), rhodamine B (RhB), and tetracyclines (TC). Moreover, under the optimized carbonization temperature (Tc) of 300 °C, the TiO2−x/CBC-300 exhibited an outstanding separation efficiency of 97.07% for the MB/MO solution. Detailed analysis confirmed that Tcwas a key regulator for adjusting the Voconcentration, which directly influenced the surface charge density and, further, the separation efficiency of TiO2−x/CBC. Additionally, the used adsorbent could be easily regenerated from washing by ethanol. After 4 regenerations, the adsorption efficiency declined only by 6.9% after 20 min and 13.6% after 120 min adsorption, respectively. Ultimately, this oxygen vacancy-rich TiO2−x/BC system illuminated good prospects for mixed dye wastewater adsorption and separation.
研究领域:
环境科学
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材料科学
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高影响因子
Small
·
2021
·Vol. 18
·期 6
·2103528
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IF 13.281
Bijiang Geng,Shuang Xu,Ping Li,Xiaokai Li,Fuling Fang,Dengyu Pan,Longxiang Shen
Sonodynamic therapy as a promising noninvasive modality is being developed for tumor therapy, but there is a lack of next-generation sonosensitizers that can generate full ROS at high yields and simultaneously deplete elevated levels of glutathione (GSH) in tumor cells. Semiconductor p-n junctions are engineered as high-efficacy sonosensitizers for sonodynamic tumor eradication using pyridine N-doped carbon dots (N-CDs) as a p -type semiconductor and oxygen-deficient TiO 2− x nanosheets as a n -type semiconductor. The rate constants of 1 O 2 and •OH generation by ultrasound-excited N-CD@TiO 2− x p-n junctions are 4.3 and 4.5 times higher than those of TiO 2 , respectively. A Z-scheme carrier migration mechanism in the p-n junction achieving the rapid spatial separation of the ultrasound-generated electron–hole pairs for enhanced full ROS production is proposed. GSH-cleavable, Pt-crosslinked, N-doped CD fluorescent probes to detect the presence of intracellular GSH are also constructed. A GSH-responsive, p-n junction platform (Pt/N-CD@TiO 2− x ) with integrated GSH detection, GSH depletion, and enhanced sonodynamic performance is then assembled. Malignant tumors are completely eradicated without relapse via intravenous administration of low-dose Pt/N-CD@TiO 2− x under ultrasound irradiation. This work substantiates the great potential of biocompatible, GSH-responsive p-n junctions as next-generation sonosensitizers via p-n junction-enhanced ROS generation and metal ion oxidation of intracellular GSH.
研究领域:
生物医学工程
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肿瘤学
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材料科学
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高影响因子
ACS Nano
·
2025
·
IF 16
Weihao Zhu,Yabing Sun,Kaiwei Xu,Chaoxiang Xie,Ming Yang,Yonglong Ye,Jiayong Luo,Haijing Cui,Liangxue Lai,Tianxiang Chen,Xuehua Ma,Jie Lin,Wenzhi Ren,Aiguo Wu
The clinical translation of inorganic sonosensitizers for cancer sonodynamic therapy (SDT) is constrained by two interconnected barriers: insufficient therapeutic efficacy due to low reactive oxygen species (ROS) yield and long-term toxicity risks due to poor metabolic clearance. Although conventional ultrasmall size designs achieved renal clearance, they reduce the sonosensitizers’ accumulation in the tumor and further weaken treatment outcomes. To address these challenges, we developed a tumor microenvironment (TME)-responsive Mn-doped TiO2–x nanoplatform (2.4 nm). Optimal Mn doping induced defect-mediated bandgap narrowing, generating oxygen vacancies and intermediate states that reduced the TiO2 bandgap from 3.20 to 2.30 eV, thereby enhancing sonosensitivity. Simultaneously, Mn2+-driven Fenton-like catalysis exploited elevated H2O2 levels to generate O2 in the TME, alleviating tumor hypoxia while amplifying ROS production. Critically, pH-triggered surface transformation enabled spontaneous intratumoral aggregation: acid-labile PEG shedding exposed biorthogonal click groups that cross-link sonosensitizers into ∼230 nm assemblies, thereby boosting tumor retention. This integrated strategy elevated cellular ROS yield 9.7-fold under ultrasound irradiation and achieved 98.2% tumor suppression in mouse models. Concurrently, nonaccumulated sonosensitizers were cleared by the kidney due to their ultrasmall diameter, mitigating systemic toxicity risks. This work establishes a paradigm for inorganic sonosensitizers that intrinsically unite defect-optimized sonosensitivity, TME-enhanced catalysis, and tumor-retentive aggregation with on-demand metabolic clearance, resolving the fundamental efficacy–safety conflict in SDT.
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Mengqin Zhou,Xiu Wan,Xia Zhang,Xiaoxuan Wang,Shixiong Hao,Lei Li,Chunru Cheng,Jian Peng,Yongfan Wang
Green synthesis of OV-rich TiO 2- x using L-cysteine, avoiding hazardous H 2 /NaBH 4. • Construction of hollow BiOI/ TiO 2- x S-scheme heterojunction via in-situ assembly. • Hollow structure, OVs, and S-scheme synergistically boost light harvesting & charge separation. • 94.24% TC removal in 120 min; kinetic constant 3.83–7.97 times higher than controls. • •O 2 − and h + as dominant active species; S-scheme mechanism confirmed. Addressing the challenge of tetracycline (TC) contamination in aquatic environments, this work reports a high‑performance S‑scheme photocatalyst fabricated via a green and sustainable strategy. Oxygen vacancy (OV)‑rich TiO 2- x hollow microspheres were prepared by a hard‑template method using L‑cysteine as a green reductant, followed by in‑situ hydrothermal deposition of BiOI nanosheets. The optimized BiOI/TiO 2- x -5% composite exhibits 94.24% TC degradation within 120 min under visible light, with a reaction rate constant 3.83, 3.67, and 7.97 times higher than those of pristine TiO 2 , TiO 2- x , and BiOI, respectively. The boosted performance stems from the synergistic effects of the hollow structure, which enhances light harvesting and mass transfer, and the OV‑mediated S‑scheme heterojunction, which greatly suppresses charge recombination while retaining strong redox potentials. Mechanistic investigations confirm •O 2 − and h + as the dominant active species. This work provides a promising paradigm for designing efficient defect‑mediated hollow heterojunctions toward sustainable antibiotic wastewater remediation. Download: Download high-res image (164KB) Download: Download full-size image
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