APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Yangjun Luo,Yanwei Wang,Youyuan Wang,Heming Huang,Li Zhang,Huijuan Zhang,Yu Wang
Although various alloys have been extensively explored to enhance catalyst activity and stability in oxygen reduction, degradation of performance due to long-term operation has plagued the crowd. Here, we develop a catalyst synthesis strategy based on the coexistence of monoatomic Fe and Pt-based clusters/alloys on NC/TiO x . Fe/PtCo-NC/TiO x exhibits a half-wave potential of 0.948 V and mass activity of 3.69 A mg Pt −1 at 0.9 V, the latter being approximately 32.1 times higher than that of 20% Pt/C (0.115 A mg Pt −1 ). Additionally, it also shows maximum power densities of 952.2 mW cm −2 and 215.8 mW cm −2 in the H 2 /O 2 fuel cell and Zn-air battery, respectively. The combination of illumination and calcination promotes the electron transfer between Pt and TiO x , thus enhancing the catalytic activity and stability. We also explore the approach and mechanism of using illumination to suppress catalyst performance degradation. The intermittent irradiation inhibits the dissolution of Pt to facilitate the Fe/PtCo-NC/TiO x durability beyond that of most reported metal catalysts, with a half-wave potential degradation of only 14 mV after 30,000 cycles. The ingenious use of illumination provides a simple and feasible strategy for the sustainable utilization of catalysts.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
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IF 15.7
Zhang Kexin,Liang Xiao,Wang Yucheng,Zou Yongcun,Zhao Xiao,Chen Hui,Zou Xiaoxin
The dynamic reconstruction of oxygen evolution electrocatalysts dictates their performance, yet conventional Ir-based materials face an inherent activity-stability trade-off due to surface amorphization into hydrous IrO x phases accompanied by lattice oxygen mechanisms. Here, we uncover a distinct reconstruction pathway for supported Ir nanoparticles, where a TiO x @Ti substrate drives a bulk phase transition from metallic Ir to crystalline rutile IrO 2 during electrocatalysis. Unlike surface-limited amorphization, this support-guided crystallization shifts the reaction mechanism from involving lattice oxygen mechanism to the complete adsorbate evolution mechanism, as confirmed by mechanistic and structural analyses. Consequently, the Ir/TiO x @Ti catalyst achieves both high activity and durability in acidic media, demonstrated in three-electrode systems and proton exchange membrane water electrolyzers. This work redefines support roles in electrocatalyst reconstruction, demonstrating that bulk phase engineering—rather than surface modification—resolves the long-standing efficiency-durability conflict in acidic oxygen evolution.
研究领域:
电化学
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催化
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材料科学
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纳米技术
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能量转换
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ACS Catalysis
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2024
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IF 11.3
Chenfan Gong,Hao Wang,Jian Zhang,Chengguang Yang,Xianni Bu,Haiyan Yang,Jiong Li,Peng Gao
Hydrogenation of CO2 to ethanol is an efficient process for the utilization of CO2 along with the production of value-added chemicals. However, CO2 hydrogenation to ethanol is a complicated reaction, requiring the catalyst to activate CO2 efficiently and accurately regulate the C–C coupling to achieve a high ethanol selectivity simultaneously. Herein, we report the synthesis of RhFeOx catalysts supported on TiO2 with different crystal phase compositions (anatase, rutile, and P25), which were applied for the selective CO2 hydrogenation to ethanol. The RhFeOx/P25 catalyst presented a high dispersion of Rh nanoparticles on the P25 support with abundant Rh0–Rhδ+–OV–Ti3+ (OV: oxygen vacancy) interfacial sites over the anatase/rutile junction. The optimized RhFeOx/P25 catalyst exhibited a high ethanol space–time yield of 18.7 mmol gcat–1 h–1 and a high Rh turnover frequency of 544.8 h–1 with 90.5% ethanol selectivity. An in-depth investigation via various ex situ and in situ characterizations as well as H2/D2 exchange and C2H4 pulse hydrogenation experiments demonstrated that the Rh0–Rhδ+–Ov–Ti3+ interfacial sites played a crucial role in the conversion of CO2 to ethanol. The surface Rh0 sites facilitated the CO2 activation and hydrogenation, while the Rh0–Rhδ+–Ov–Ti3+ interfacial sites boosted the C–C coupling to produce ethanol. The high-performance RhFeOx/P25 catalyst also provides an attractive route for highly efficient ethanol synthesis via CO2 hydrogenation.
研究领域:
催化化学
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环境科学
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材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Xiaowei Wu,Le Hu,Ting Zhao,Xingyi Hu,Pu Hu,Junlong Feng,Chaoqun Shang
A BTO-TiO x /Bi-NC interlayer enables synergistic Li + regulation and guidance. • Li||Li cells achieve 800 h stable cycling in high-voltage ester electrolyte. • Li− S batteries retain 466.53 mAh g −1 after 400 cycles at 3C in ether electrolyte. The practical application of Li metal anodes is hindered by uncontrollable dendrite growth, which stems from the unstable solid electrolyte interphase (SEI) and heterogeneous Li + flux. Herein, we report a porous Bi 4 Ti 3 O 12 (BTO) decorated with in-situ generated titanium oxide and bismuth nanocrystals (denoted as BTO-TiO x /Bi-NC) composite, as a multifunctional interfacial layer to address these challenges. The integrated TiO x ensures high ionic conductivity, while Bi-NC effectively regulate Li + flux, thereby guiding uniform Li + plating/stripping. Moreover, it is hypothesized that the reversible Li 3 Bi alloying reaction during cycling could provide additional nucleation sites, potentially contributing to enhanced Li deposition homogeneity. Benefiting from this rational design, BTO-TiO x /Bi-NC promises the symmetric Li||Li cell exhibiting remarkable stability for 800 h at 1 mA cm −2 in high-voltage ester-based electrolyte. When coupled with an S cathode, the full Li S battery maintains a discharge capacity of 466.53 mAh g −1 after 400 cycles at 3C in ether-based electrolyte, demonstrating excellent long-term cyclability. This work proposes a promising strategy for stabilizing Li metal anodes via combined Li + flux regulation and alloying chemistry, paving the way for durable high-energy-density batteries. Download: Download high-res image (145KB) Download: Download full-size image
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Jie Xu,Hongji Li,Huimin Feng,Yuqin Ma,Dandan Wang,Jianwei Zhu
The removal of refractory organic contaminants in the environment is vital, but developing highly active catalysts with a simple synthesis process remains a challenge. Herein, NH 2 -MIL-125(Ti) (Ti-MOF) as a template, Ti 3+ -TiO x clusters of different quantities were embedded in the CdIn 2 S 4 nanosheets to construct Ti 3+ -TiO x /CdIn 2 S 4 (TiCIS) heterojunction by an in-situ self-assembly strategy, which had a hollow structure, strong visible light absorption, high separation rate of carriers, and more active sites. During the degradation experiment of Rhodamine B (RhB), TiCIS25 exhibited the best photocatalytic performance, and 98.0% of RhB was degraded within 60 min of visible irradiation. The intermediates in the RhB degradation and their ecotoxicity were analyzed, which revealed that RhB degradation was a detoxification process. The radical trapping experiments and electron spin resonance (ESR) tests indicated that e - , 1 O 2 , and ·O 2 - are the main active species for RhB degradation. Moreover, a possible photocatalytic mechanism was proposed based on electrochemical tests. The photodegradation performance of the as-prepared TiCIS catalyst under different reaction parameters (authentic water matrices, initial pH, coexisting anions, organic matter concentration, actual sunlight, reaction temperature, and multiple pollutants) and circulating experiments, as well as the photo-reduction process CO 2 , reflected that TiCIS25 possessed excellent practicability, cyclic stability, and universal applicability. Above all, TiCIS25 exhibited great potential in photocatalytic processes, and the work provided a feasible strategy for designing high-performance photocatalysts .
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 11
·2213961
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IF 19
Linghui Zhang,Chao Fu,Shi Wang,Minhuan Wang,Ruiting Wang,Shengling Xiang,Zhiyong Wang,Jing Liu,Hongru Ma,Yudi Wang,Ying Yan,Min Chen,Lei Shi,Qingshun Dong,Jiming Bian,Yantao Shi
Flexible perovskite solar cells (f-PSCs) show great promise in portable-power applications (e.g., chargers, drones) and low-cost, scalable productions (e.g., roll-to-roll). However, in conventional n–i–p architecture f-PSCs, the low-temperature processed metal oxide electron transport layers (ETLs) usually suffer from high resistance and severe defects that limit the power conversion efficiency (PCE) improvement of f-PSCs. Besides the enhancement in the mobility of metal oxide and passivation for perovskite/ETL interfacial defects reported in previous literature, herein, the electron transport loss between the metal oxide nanocrystallines within the ETL is studied by introducing an amorphous F-doped TiO x (F-TiO x ) caulked crystalline SnO 2 composite ETL. The F-TiO x in this novel composite ETL acts as an interstitial medium between adjacent SnO 2 nanocrystallines, which can provide more electron transport channels, effectively passivate oxygen vacancies, and optimize the energy level arrangement, thus significantly enhancing the electron mobility of ETL and reducing the charge transport losses. The composite ETL-based f-PSCs achieve a high PCE of 22.70% and good operational stability. Furthermore, a moderate roughness of the composite ETL endows f-PSCs with superior mechanical reliability by virtue of a strong coupling at the ETL/perovskite interface, by which the f-PSCs can maintain 82.11% of their initial PCE after 4000 bending cycles.
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Surfaces and Interfaces
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2024
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IF 5.7
Jingting Su,Junyi Xia,Huijun Liang,Jun Xiao,Ruohu Zhang,Shuhong Xu,Li Zhu
Amorphous materials have recently garnered significant interest due to their low-cost fabrication methods, extensive surface area and plentiful surface defects , which offer numerous active sites for catalytic reactions . However, carriers self-trapping and recombination caused by bulk defects limit the employment of amorphous materials as photocatalysts . As such, it is essential to adjust the structure and defects to improve carriers utilization for creating high-performance amorphous photocatalysts. In this study, we developed a novel and facile strategy to fabricate a quasi-2D amorphous crepe-like TiO x -Au (cTiO x -Au) photocatalyst, in which the cTiO x was synthesized simply through one-step hydrolysis method at room temperature by constructing discrete reaction system with mass-confinement of the precursor to guide the morphology of the cTiO x . The removal efficiencies of the cTiO x -Au to antibiotic tetracycline (TC) and gaseous pollutant formaldehyde (HCHO) under visible light were 84.43 % and 95.92 %, respectively, which greatly surpassed those of its counterparts, normal amorphous TiO x (amTiO x )-Au (54.32 % and 73.67 %) and crystalline catalyst TiO 2 -P25-Au (49.29 % and 54.03 %). The remarkable visible-light photocatalytic capacity of cTiO x -Au can be attributed to the unique quasi-2D morphology of cTiO x . The ultrathin nanostructure not only maximizes surface defects and minimizes bulk defects, but also effectively shortens the carriers transport time and reduces recombination probability, on the other hand, it provides ample adsorption sites and accessible binding sites for plasmonic Au nanoparticles to amplify the effect of surface plasmon resonance enhancement. The excellent photocatalytic performances of cTiO x -Au for removing both aqueous and atmospheric pollutants endow it great potential in real environmental remediation applications.
研究领域:
材料科学
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环境科学
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Youpei Wang,Xiang Zheng,Shiyun Liang,Danyan Wang,Xiaojun He,Lingxia Pang
Traditional treatments for drug-resistant bacterial keratitis and pneumonia often prove ineffective due to the presence of biofilm barriers and multidrug resistance. Existing nano-antibacterial systems face several limitations, including insufficient tissue penetration depth in the first near-infrared (NIR I) window, the inability of a single treatment modality to simultaneously disrupt biofilms and eradicate residual bacteria, and a lack of efficacy validation in cross-organ (ocular-pulmonary) infection models. In this study, we employed a defect engineering strategy, to construct a palladium-doped TiO 2 nanozyme with oxygen vacancies (PdO V -TiO X ). This nanozyme achieves multiple antibacterial effects through the synergistic combination of second near-infrared (NIR-II) laser-activated photothermal therapy and chemodynamic therapy. Under 1064 nm laser excitation, the system utilizes oxygen vacancy-enhanced peroxidase-like activity to continuously generate hydroxyl radicals (•OH), resulting in a 5.2-fold increase in radical production compared to dark conditions. Additionally, it induces a local temperature rise (ΔT = 28.2 °C). These combined effects—physical disruption of the biofilm matrix and ROS-mediated oxidative stress—effectively dismantle the defense mechanisms of drug-resistant bacteria. In models of drug-resistant Staphylococcus aureus keratitis and pneumonia, PdO V -TiO X demonstrated therapeutic efficacy in both the eye and lung, indicating the broad cross-organ applicability of this treatment. Under NIR-II irradiation, the PdO V -TiO X nanozyme significantly elevated ROS levels at the infection site, achieving efficient bactericidal action while effectively penetrating and disrupting mature biofilms. This work presents a novel defect-engineering-regulated nanozyme synergistic therapeutic strategy for the treatment of multidrug-resistant bacterial infections.
研究领域:
纳米医学
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抗菌治疗
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材料科学
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生物医学工程
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传染病学
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Journal of Energy Chemistry
·
2022
·
IF 13.599
Hao Li,Liqun Wang,Nan Li,Jianmin Feng,Feng Hou,Sihui Wang,Ji Liang
Electrocatalytic nitrogen reduction reaction (eNRR) at the ambient conditions is attractive for ammonia (NH 3 ) synthesis due to its energy-efficient and eco-friendly features. However, the extremely strong N≡N triple-bonds in nitrogen molecules and the competitive hydrogen evolution reaction lead to the unsatisfactory NH 3 yield and the Faradaic efficiency (FE) of eNRR, making the development of high-performance catalysts with adequate active sites and high selectivity essential for further development of eNRR. Addressing this, we herein report a Bi and K dual-doped titanium oxide (BTO@KTO) material, which is prepared by a cation exchange reaction between K 2 Ti 4 O 9 and molten BiCl 3 , for high-performance eNRR catalysts. Benefiting from the controllable molten-salt cation exchange process, a highly active surface containing Bi/K sites and rich oxygen vacancies has been obtained on titanium oxide. Under the synergy of these two merits, an efficient eNRR catalysis, with the NH 3 yield rate of 32.02 μg h −1 mg cat. −1 and the FE of 12.71%, has been achieved, much superior to that of pristine K 2 Ti 4 O 9 . This work thus offers a high-performance electrocatalyst for eNRR, and more importantly, a versatile cation-exchange strategy for efficiently manipulating materials' functionalities.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Guolong Qiu,Wei He,Guangxu Yao,Chuanzhen Feng,Huijuan Zhang,Jinling Ma,Yu Wang
Development of non-noble metal-based electrocatalysts to enhance the performance of zinc-air batteries (ZABs) is of great significance, but it remains a formidable challenge due to their poor stability and activity. Herein, a bifunctional CuNi-TiO x /NCNFS electrocatalyst , featuring with electron-rich copper-nickel (CuNi) alloy nanoparticles anchored on titanium oxide/ N -doped carbon nanofibers (TiO x /NCNFS), is constructed by a dual-substrate loading strategy. The introduction of TiO x has led to a significant increase in the stability of the dual-substrate. The strong electronic interaction between CuNi and TiO x strengthens the anchoring of active metal sites, thus accelerating the electron transfer. Theoretical calculations unclose that NCNFS can regulate the charge distribution of TiO x , inducing the charge transfer from NCNFS → TiO x → CuNi, thereby reducing the d-band center of Cu and Ni, which is beneficial to the desorption of intermediate oxide species of the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Therefore, CuNi-TiO x /NCNFS delivers a remarkable bifunctional performance with a low OER overpotential of 258 mV at 10 mA cm −2 and an ORR half-wave potential of 0.85 V. When assembled into ZABs, CuNi-TiO x /NCNFS shows a low potential gap of 0.64 V, a higher power density of 149.6 mW cm −2 at 330 mA cm −2 , and an outstanding stability for 250 h at 5mA cm −2 . This study provides a novel approach by constructing dual-substrate to tune the electronic structure of active metal sites for efficient rechargeable ZABs.
研究领域:
材料科学
·
能源化学
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Materials Research Express
·
2019
·Vol. 6
·期 7
·076430
·
IF 1.449
Ying Tao,Daocheng Pan
Transparent conductive thin films play an important role in antistatic coating. In this work, highly robust Ag nanowires/TiOx hybrid transparent conductive thin film was deposited by a one-step and low-temperature method. Firstly, 4.2 g of silver nanowires and 1.0 liter of TiOx sol-gel solution were synthesized. The Ag nanowire dispersion and TiOx sol-gel solution were mixed and sprayed onto many types of substrates, including glass, wood and marble. Highly robust Ag nanowires/TiOx hybrid thin film with a sheet resistance of 7–102*/□ and transmission of 63%–84% can be obtained by a low-temperature sintering process or by UV/ozone irradiation at room temperature. Our results indicated that low-cost and robust Ag nanowires/TiOx hybrid thin films have a high potential in antistatic coating.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Hainan Shi,Jun Du,Haozhi Wang,Zhenghao Jia,Dingfeng Jin,Jiaqi Cao,Jungang Hou,Xinwen Guo
Solar-driven CO 2 conversion into fuels is a promising solution toward green energy conversion. It is a challenge to regulate the precise structure of photocatalysts at the atomic scale, facilitating the charge transfer and improving CO 2 photoreduction performance. Herein, conductive Ti 3+ -rich TiO x clusters with unsaturated Ti–O 5 coordination incorporated into nanosheets-assembled hollow sulfide semiconductors were prepared through a versatile transformation strategy by using NH 2 -MIL-125(Ti) metal–organic–framework as precursor. This typical photocatalysts exhibit highly selective photoreduction of CO 2 , achieving a super high visible-light photocatalytic CO evolution activity of 1100 μmol g −1 h −1 . The active sites were identified on the surface of conductive TiO x clusters, inducing efficient trapping of photogenerated electrons at the interface and suppressing H 2 generation. This enhanced performance is ascribed to Ti 3+ -rich TiO x clusters as an efficient cocatalyst on sulfide semiconductor providing more active sites due to electrical conductivity and unsaturated coordination environment. This work provides a promising approach to enhance photocatalytic performance of the catalysts coupled by unique metal oxide clusters for selective photoreduction of CO 2 .
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