Advanced Sustainable Systems
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2026
·Vol. 10
·期 2
·e01682
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IF 5.6
Handuo Fu,Ke Fang,Shenhui Ma,Lin Wang,Yuyu Bu
In theory, the utilization of a Z-scheme photogenerated carrier transport system has the potential to significantly enhance the photogenerated voltage for photoelectrochemical overall water splitting. However, thus far, there have been no previous reports on such phenomena with silicon-based semiconductor photoelectrodes. In this study, we fabricated an n-Si/Pt/Mo-doped BiVO 4 (Mo: BVO) sandwich-like film with an intermediate carrier transfer layer to prepare a silicon-based photoelectrode with an indirect Z-scheme system. Additionally, by leveraging the lattice distortion effect over Mo: BVO, we increased the fusion ability of the sandwich-like interface between different substances. For the first time, we achieved generation of anodic displacement current via negative voltage (−0.57 V (vs. RHE)), resulting in a photocurrent density of 1.56 mA/cm 2 and a photogenerated voltage five times higher than that of the n-Si/Mo: BVO structure. Through combining experimental approaches with theoretical calculations, it has been confirmed that this realization is attributed to the contribution of the transport process within the Z-scheme system in the n-Si photoelectrode. Furthermore, milliampere-level photocurrent under negative bias was observed for the first time on an n-Si photoelectrode, providing a novel approach for constructing silicon-based photoelectrodes for overall water splitting.
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CHINESE JOURNAL OF CATALYSIS
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2026
·
IF 17.2
Yun Huang,Qi Chen,Yueling Chen,Zefeng Yang,Jionghua Wu,Jimmy C. Yu,Ling Wu
The generation of active hydrogen species (H*) is an essential step in the photocatalytic conversion of nitrogen molecules (N 2 ) to ammonia (NH 3 ). Metal-organic frameworks (MOFs) are versatile porous structures but they do not exhibit sufficient photocatalytic activities for nitrogen fixation. Adding appropriate amounts of noble metal species as a cocatalyst to MOFs can often improve their activities. This work uses a photoreduction strategy to reduce the right amount of Pt 4+ to Pt clusters, and confines the remaining Pt 4+ uniformly onto DUT-67(Zr). This is realized by taking advantage of a unique Pt-S electron channel, and the unsaturated Zr sites are concurrently in-situ generated under light exposure. The unsaturated Zr sites adsorb and activate N 2 , while the Pt clusters are involved in the water splitting process on DUT-67(Zr) to generate more H*, leading to continuous H* supply that would speed up the catalytic hydrogenation of nitrogen intermediate NH x . The Pt-S electronic channel formed between highly dispersed single atoms Pt and DUT-67(Zr) facilitates the separation and transfer of photo-generated charge carriers. Consequently, with the synergistic effect of unsaturated Zr sites, Pt clusters and Pt-S electron channels, a high photocatalytic nitrogen fixation performance of 78.8 μmol g ‒1 h ‒1 can be achieved. This is 10.4 times higher than that of the sample DUT-67-L with only unsaturated Zr sites and no Pt loading. This work provides an insight to rational design of uniform dispersed precious metal-based MOF photocatalyst for efficient photocatalytic ammonia synthesis.
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TRANSACTIONS OF TIANJIN UNIVERSITY
·
2026
·
IF 7.8
Gong Mengcong,Wang Qingfa,Liu Linlin,Zhang Xiangwen
ZSM-48 zeolite, which features one-dimensional ten-membered-ring straight channels, is an ideal support for hydroisomerization catalysts to improve fuel low-temperature fluidity. To improve the poor low-temperature fluidity of Fischer–Tropsch synthesis products, this study employed Mg modification on Pt/ZSM-48 catalysts to optimize their hydroisomerization performance. A series of Mg-Pt/ZSM-48 catalysts with varying Mg loadings was prepared via incipient wetness impregnation. The effects of Mg modification on the pore structure, acidity, and metal–acid balance of the Pt/ZSM-48 catalyst system were systematically investigated. Catalytic performance was evaluated using n-hexadecane as a model compound. The Mg species selectively modified the micropore channels, decreasing the specific surface area and micropore volume. Moreover, Mg 2+ selectively neutralized Brønsted acid sites, reducing the concentration of medium-strong acid sites and Brønsted acidity while introducing Lewis acid sites, thereby lowering the Brønsted/Lewis acid ratio. Appropriate Mg modification optimized the metal–acid balance, making acid-catalyzed skeletal isomerization the rate-determining step. Although the Mg-modified catalysts exhibited moderately reduced catalytic activity, their isomer selectivity and yield were significantly enhanced. The 0.5 Mg-Pt/Z48 catalyst achieved an isomer yield of 81.81% at 91.18% conversion, representing a 9% improvement over the unmodified catalyst. The micropore confinement effect weakened the interaction between alkane molecules and micropore channels, promoting the key–lock catalytic mechanism. This increased the formation of mono-branched isomers close to the center of the main carbon chain, significantly improving the low-temperature fluidity of the fuel. This study provides a simple and efficient strategy for designing high-performance hydroisomerization catalysts for long-chain n-alkanes. Graphical
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Nature Communications
·
2026
·
IF 18.1
Wang Zixu,Zhang Binbin,Ding Jinyu,Tao Yunlong,Sun Lichao,Zhang Qingfeng
Spin selection in chiral nanocatalysts enabled by the chiral-induced spin polarization (CISS) effect has emerged as a promising strategy for boosting the performance of the oxygen reduction reaction (ORR). However, achieving atomic-scale control of catalytically active surfaces on chiral nanostructures remains challenging. Herein, we demonstrate an approach for the atomic-level engineering of Pt shells on chiral substrates to enhance ORR performance. Pt shells with controlled thicknesses are deposited on chiral Au nanoparticles through a combined protocol of cyclic underpotential deposition and galvanic replacement reaction. This strategy not only maximizes the atomic utilization efficiency of Pt but also preserves the chiral geometry of the substrate and its chiroptical activity. For the chiral Au@Pt nanocatalysts, a volcano-type relationship is observed between the Pt shell thickness and ORR performance. The chiral Au@Pt nanoparticles exhibit a capability of spin polarization due to the CISS-like effect and competitive ORR activities. This work establishes a route for fabricating catalytically active chiral nanocatalysts with CISS-like effects, thereby laying a foundation for the development of advanced spin-selective electrocatalysts.
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Science China-Chemistry
·
2025
·
IF 9.7
Wang Xianhui,Chen Sai,Sun Guodong,Chang Xin,Tian Kaige,Zhao Zhenyi,Wu Zelin,Fu Donglong,Zhao Zhi-Jian,Pei Chunlei,Gong Jinlong
Supported-metal catalysts are well-established for industrial catalysis, but controlling the metal-oxide interaction (MSI) is challenging because of the intricate geometric and electronic effects. Herein, this paper describes the strategy of controlling metal-oxide interaction by pre-tailoring the oxygen vacancy (O v ) concentrations on defective metal oxides for supported Pt catalysts. ZnO distinguishes itself among the metal oxides examined, with the structural and chemical attributes of O v playing a pivotal role in determining its effectiveness. At lower O v concentration (less than 0.82 mmol/g ZnO ), the O v in defective ZnO x impedes Pt growth, while higher O v concentration (0.82 to 5.63 mmol/g ZnO ) induces an electron-sufficient Pt state without compromising Pt dispersion. During propane dehydrogenation (PDH), performed under reducing conditions, the optimized Pt/ZnO x achieved 44% of propane conversion and 90% of propylene selectivity at 600 °C under 4 h −1 of C 3 H 8 , which is comparable to that of PtSn/Al 2 O 3 analogue. This oxygen vacancy engineering strategy provides mechanistic insights into disentangling geometric and electronic factors, advancing the rational design of MSI-controlled PDH catalysts.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Ying Xu,Kang Xue,Furong Li,Chang Song,Minhua Ai,Zehao Han,Chengxiang Shi,Ruijie Gao,Zhen-Feng Huang,Xiangwen Zhang,Lun Pan,Ji-Jun Zou
Methylcyclohexane (MCH) / toluene (TOL) system is considered as a promising candidate for large-scale green hydrogen storage, and the catalytic MCH dehydrogenation is the key reaction for the effective system recycling. As the important property, the electronic structure of Pt active sites determines the dehydrogenation dynamics, but the mechanism for its effect on dehydrogenation is still ambiguous. Herein, we proposed a support (CeO2) facet mediated method to rationally regulate metal-support interaction as well as d-orbital electron occupation of Pt sites for efficient MCH dehydrogenation. The characterizations indicate the interfacial Pt-O coordination numbers are reduced from Pt/CeO2 (110) to Pt/CeO2 (111) and Pt/CeO2 (100), leading to the gradually decreased interfacial charge transfer and metal-support interaction (MSI). The in-situ characterization of catalytic reactions and DFT calculation results confirm the rate-limiting step of dehydrogenation is the desorption of products H2 and TOL. The MCH dehydrogenation performances show the catalytic activities of Pt/CeO2 (111) > Pt/CeO2 (110) > Pt/CeO2 (100). Notably, Pt/CeO2 (111) with moderate MSI induces a moderate eg-orbital electron occupation of Pt-O-Ce sites to accelerate H2 formation and desorption, while the resulted least t2g-orbital electron occupation of Pt-Pt sites weakens TOL adsorption, therefore showing the best TOL yield of 91.2% at 350 °C and WHSV of 4.62 h-1. This work reveals the mechanism of support-facet-mediated d-orbital electron occupation regulation of Pt sites, which provides a guidance for the rational design of highly efficient dehydrogenation catalysts.
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Materials Today Chemistry
·
2025
·
IF 6.7
Cijun Shuai,Jiang Xiao,Kangdong Wang,Gao Pan,Shuping Peng,Qi Zhong
Diabetic patients frequently suffer from skin ulcers exacerbated by bacterial infections. Cu 2 O nanozymes present a promising antibacterial alternative to antibiotics due to their enzyme-like catalytic activity. However, their efficacy is hindered by the low H 2 O 2 concentration in the bacterial microenvironment and the slow electron transfer during catalysis. To mitigate these limitations, we exploited Cu 2 O's intrinsic reducing ability to grow Au–Pt nanoparticles, thereby creating Cu 2 O@Au–Pt nanoreactors. Subsequently, we fabricated Cu 2 O@Au–Pt/Polycaprolactone skin scaffolds using laser powder bed fusion. In the scaffold, Cu 2 O catalyzed H 2 O 2 to produce hydroxyl radicals, inducing bacterial apoptosis. Au–Pt nanoparticles enhanced this catalysis in three manners: by providing additional H 2 O 2 through glucose oxidation, elevating the reaction temperature via plasmonic resonance, and facilitating electron transfer through metal-support interactions. Photothermal experiments and simulations illuminated the near-field coupling and interface hotspot formation mechanisms in the Cu 2 O@Au–Pt hybrid structure, boosting the catalytic rate at the interface. DFT calculations and electrochemical tests verified a reduced energy barrier for electron transfer in the Cu 2 O@Au–Pt system, enhancing its redox capability. Upon NIR irradiation, the scaffold increased intracellular ROS by 84.5 % and achieved a 99.9 % antibacterial efficacy against E. coli. These findings highlight the potential of the Cu 2 O@Au–Pt nanozyme scaffold for treating diabetic wounds.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
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IF 3.141
Ying Huo,Xuyu Wang,Zebao Rui,Xiaoqing Yang,Hongbing Ji
Insight into the relationship between catalytic trends and physicochemical properties of composite nanoparticles is essential for their rational design. Herein, a series of 3d-M (M = Mn, Fe, Co, Ni) metal hydroxide-promoted PtM(OH)x/Al2O3 catalysts are developed and well characterized for establishing the catalytic HCHO oxidation reactivity trend as a function of more fundamental properties, such as hydroxyl concentration and adsorption strength. The reactivity of PtM(OH)x/Al2O3 exhibits an increasing trend of Mn < Fe < Co < Ni, which is governed by their OH–M2+δ bond strength (Ni < Co < Fe < Mn) and surface hydroxyl concentration (Mn < Fe < Co < Ni). Both PtCo(OH)x/Al2O3 and PtNi(OH)x/Al2O3 exhibit a (>)95% HCHO conversion and (>)100 h performance stability at 30 °C with a low 0.2 wt % Pt loading amount. The identification of these catalytic trends provides foundations for composite active sites design for HCHO oxidation and other hydroxyl-involved reactions.
研究领域:
催化化学
·
材料科学
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ACS Applied Materials & Interfaces
·
2019
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IF 8.456
Yangping Zhang,Fei Gao,Caiqin Wang,Yukihide Shiraishi,Yukou Du
Engineering robust electrocatalysts is always a key point in direct alcohol fuel cells. Catalysts with a one-dimension (1D) structure are well studied and considered as promising candidates among various catalysts in the past decades; however, the precise regulation on the surface structure of 1D nanomaterials is still a worthy subject. By creatively introducing a trimetallic nanoalloy, core@multishell structure, and 1D nanowire (NW) morphology, we have constructed a kind of novel spiny PtFePd@PtFe/Pt core@multishell 1D NW catalysts with PtFePd as the core and PtFe/Pt as the multishell on the basis of improving catalytic property. The composition-optimized Pt5FePd2 1D NWs display remarkable catalytic properties for ethanol oxidation reaction and methanol oxidation reaction, in which mass activities are 4.965 and 4.038 A mg–1, 4.6 and 5.0 and 4.0 and 9.2-fold higher than Pt/C and Pd/C catalysts. Furthermore, the obtained Pt5FePd2 NWs can also retain favorable stability after durability tests. The unique core@multishell structure, spiny 1D NWs with many steps and kinks, and interior electronic and synergistic effect all contribute to the advanced catalytic performance. The present work has rationally designed the novel 1D PtFePd@PtFe/Pt core@multishell NW catalysts and offered a meaningful guideline for the designing of high-performance electrocatalysts.
研究领域:
材料科学
·
电催化
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NANOTECHNOLOGY
·
2025
·Vol. 36
·期 24
·245501
·
IF 2.8
Ning Lian,Jiahang Huo,Wei Liu,Zhiheng Zhang,Xin Chen,Yuqing Du,Xinshou Wang,Jian Song,Gang Cheng
The detection of volatile organic compounds (VOCs), particularly acetone, is critical for applications in environmental monitoring and medical diagnostics, including diabetes detection. Conventional metal oxide semiconductor sensors face challenges such as poor selectivity, high operating temperatures, and limited stability. This study addresses these limitations by developing Pt-doped ZnO nanotubes (Pt–ZnO NTs) using a coaxial electrospinning and in-situ growth method. The process effectively incorporates ZIF-8-derived hollow ZnO structures and uniformly distributed Pt nanoparticles to enhance gas sensing performance. Key findings reveal that the 1% Pt–ZnO NTs sensor exhibits exceptional acetone sensitivity (Ra/Rg = 48.2 for 10 ppm), broad detection range (81.2 ppb–50 ppm), reduced operating temperature (240 °C), and robust selectivity against interfering gases. Advanced characterization and theoretical density functional theory analysis show that Pt doping increases oxygen vacancy concentration, enhances electron transport, and reduces the material's band gap, contributing to superior sensing capabilities. Additionally, the sensor demonstrates excellent stability, repeatability, and practical applicability in distinguishing diabetic and healthy exhaled breath samples. This research introduces a novel gas sensing platform that integrates metal–organic framework-derived structures and noble metal catalysts, offering significant advancements in sensitivity, selectivity, and reliability for VOC detection.
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JOURNAL OF MATERIALS SCIENCE
·
2026
·
IF 4.4
Lu Mengqi,Wang Ruoyu,Miao Xiaoxuan,Tang Tingting,Hu Wenfeng,Jin Xiaoxuan,Wang Haoxiang,He Yuyang,Wang Yang,Xu Dongpo
The increasing consumption of high-protein seafood has heightened the demand for efficient detection of triethylamine (TEA), a key spoilage biomarker. In this study, a novel ternary SnO 2 -Pt/Ti 3 C 2 T x composite was for the first time fabricated via a combined strategy of electrospinning and electrostatic self-assembly for TEA sensing. Characterization confirmed the formation of a well-defined ternary heterostructure with abundant mesopores and a synergistic microstructure. Benefiting from this rational design, gas sensing tests revealed that the composite exhibits a high response, fast response/recovery, excellent cycling/long-term stability, and high selectivity with a low detection limit of 0.05 ppm at an optimal temperature of 122.28°C, alongside stable performance under 30–70% relative humidity. The enhanced performance is attributed to the catalytic effect of Pt, high conductivity of MXene, and synergistic interactions among the components. This work provides new insights for developing high-performance TEA gas sensors with promising practical potential. Graphical abstract
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Catalysis Science & Technology
·
2026
·
IF 4
Ruoyu Liu,Weiming Zhai,Jiahui Li,Linlin Chen,Peng Cui,Zhendong Yu,Wenshuai Zhu,Peiwen Wu
Combustion of diesel and other fuel oils releases sulfur oxides (SOx) from their inherent organosulfur compounds, causing exhaust catalyst deactivation and severe environmental pollution. Given the limitations of conventional hydrodesulfurization (HDS) in removing refractory sulfur species under mild conditions, developing efficient oxidative desulfurization (ODS) strategies has become increasingly important. To address this challenge, a supported high-entropy metal oxide catalyst, HEO(Pt)@SBA-15, was synthesized using mesoporous SBA-15 as the support and Pt in high-entropy oxide (HEO) as the primary active component. Detailed characterizations demonstatre that the high-entropy oxide was successfully confined within the mesoporous framework. The subsequent dispersion of the HEO(Pt)@SBA-15 catalyst in the ionic liquid 1-butyl-3-methylimidazolium tetrafluoroborate ([Bmim]BF4) yielded a heterogeneous ionic-liquid catalyst designated HEO(Pt)@SBA-15-B. This hybrid catalyst integrates strong extractive capability with the robust oxidation properties of the high-entropy oxide. In extractive-coupled catalytic oxidative desulfurization (ECODS) of diesel, HEO(Pt)@SBA-15-B exhibited remarkable efficiency arising from the synergistic interplay between ionic-liquid extraction and catalytic oxidation. Complete removal of dibenzothiophene was achieved within 5 h under optimized conditions, and the catalyst retained 94.2% DBT conversion after five consecutive cycles, demonstrating excellent stability and reusability.
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