JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Youyu Pang,Rui Zhang,Linjia Li,Yanhong Lin,Ziheng Li,Tengfeng Xie
The anchoring sites of metal single atoms are closely related to photogenerated carrier dynamics and surface reactions. Achieving smooth photogenerated charge transfer through precise design of single-atom anchoring sites is an effective strategy to enhance the activity of photocatalytic hydrogen evolution. In this study, Pt single atoms were loaded onto ultra-thin carbon nitride with two-coordination nitrogen vacancies (V N2c -UCN-Pt) and ultra-thin carbon nitride with three-coordination nitrogen vacancies (V N3c -UCN-Pt). This paper investigated the photocatalytic hydrogen evolution performance and photogenerated carrier behavior of Pt single atoms at different anchoring sites. Surface photovoltage measurements indicated that V N2c -UCN-Pt exhibits a superior carrier separation efficiency compared to V N3c -UCN-Pt. More importantly, the surface photovoltage signal under the presence of H 2 O molecules revealed a significant decrease. Theoretical calculations suggest that V N2c -UCN-Pt exhibits superior capabilities in adsorbing and activating H 2 O molecules. Consequently, the photocatalytic hydrogen evolution efficiency of V N2c -UCN-Pt reaches 1774 µmol g −1 h −1 , which is 1.8 times that of V N3c -UCN-Pt with the same Pt loading. This work emphasized the structure–activity relationship between single-atom anchoring sites and photocatalytic activity, providing a new perspective for designing precisely dispersed single-atom sites to achieve efficient photocatalytic hydrogen evolution.
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Catalysis Science & Technology
·
2024
·Vol. 14
·期 12
·3436-3447
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IF 4.4
Kok Bing Tan,Yiping Liu,Youting Wang,Sajid Ali,Wendong Wang,Jingru Li,Longmei Shang,Xing Yan,Xiaodong Zhang,Guowu Zhan
In this study, three different metal oxides derived from metal–organic frameworks (MOFs), including CeO2, ZrO2, and Fe2O3 were used as porous supports for loading Pt nanoparticles, and the supported catalysts (viz., Pt/CeO2, Pt/ZrO2, and Pt/Fe2O3) were evaluated for the catalytic deoxygenation of stearic acid to produce olefins by analytical pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS). Interestingly, Pt/CeO2 and Pt/Fe2O3 catalysts demonstrated high selectivity for olefins or aromatics, respectively, with alkanes as minor products, while the Pt/ZrO2 catalyst demonstrated the lowest deoxygenation efficiency. Among them, the Pt/CeO2 catalyst demonstrated the highest deoxygenation efficiency due to its highest oxygen vacancy density and the largest specific surface area (53 m2 g−1). It also demonstrated the highest selectivity for olefins (41%) due to the in situ partial formation of the bimetallic PtCe phase during the catalytic reaction at high temperature, which facilitates the decarbonylation pathway and leads to the formation of olefins as the main product. In addition, experimental optimizations of the reaction parameters were conducted on the designed Pt/CeO2 catalyst to further enhance olefin selectivity. Importantly, the Pt/CeO2 catalyst also maintained high olefin selectivity and stearic acid conversion even after six consecutive cycles. Therefore, this work has provided an alternative route to produce olefins via the decarbonylation of stearic acid over a supported Pt/CeO2 catalyst.
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Scientific Reports
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2014
·Vol. 4
·期 1
·1-6
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IF 5.078
Han Lin,Liu Hui,Cui Penglei,Peng Zhijian,Zhang Suojiang,Yang Jun
Noble metal nanoparticles with hollow interiors and customizable shell compositions have immense potential for catalysis. Herein, we present an unique structure transformation phenomenon for the fabrication of alloy Cu 3 Pt nanoframes with polyhedral morphology. This strategy starts with the preparation of polyhedral Cu-Pt nanoparticles with a core-shell construction upon the anisotropic growth of Pt on multiply twinned Cu seed particles, which are subsequently transformed into alloy Cu 3 Pt nanoframes due to the Kirkendall effect between the Cu core and Pt shell. The as-prepared alloy Cu 3 Pt nanoframes possess the rhombic dodecahedral morphology of their core-shell parents after the structural evolution. In particular, the resulting alloy Cu 3 Pt nanoframes are more effective for oxygen reduction reaction but ineffective for methanol oxidation reaction in comparison with their original Cu-Pt core-shell precursors.
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SOLID STATE SCIENCES
·
2024
·
IF 3.4
Yanping Dong,Qi Guo,Xiqiang Tian,Muhammad Zahid
The amalgamation of an appropriate cocatalyst is a proficient technique to expand the efficacy of precious Pt-based catalytic materials. In this study, Mo 2 N–TiO 2 with regularly distributed Mo 2 N particles were simply prepared for the deposition of precious Pt nanoparticles (NPs). Numerous techniques were implemented to thoroughly explore, how synthesis method influence the bulk structural, interfacial and cata1ytic features of the as-prepared 3 wt%Pt/TiO 2 and 3 wt%Pt/Mo 2 N–TiO 2 catalytic materials. The catalytic results obviously show that the 3 wt%Pt/Mo 2 N–TiO 2 catalyst has exceptional hydrogenation performance when compared to 3 wt%Pt/TiO 2 catalyst. The 3 wt%Pt/Mo 2 N–TiO 2 catalyst displayed high conversion (72.4 %) of cinnamaldehyde (CAL) with a maximum selectivity (82.1 %) towards C O bond. The excellent hydrogenation performance is attributed to the synergistic interaction taking place between Pt NPs and Mo 2 N entities of 3 wt%Pt/Mo 2 N–TiO 2 . Also, the enhanced standardized dispersal of Pt NPs on the Mo 2 N–TiO 2 surface causes more exposed Pt 0 sites on the 3 wt%Pt/Mo 2 N–TiO 2 surface, which is productive for the improved activation and conversion of C O bond of CAL to yield COL . In addition, the 3 wt%Pt/Mo 2 N–TiO 2 catalyst retained its higher catalytic activity for consecutive five successive rounds without substantial loss in either conversion or selectivity.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Zhang Tengfei,Zheng Peng,Gao Jiajian,Liu Xiaolong,Ji Yongjun,Tian Junbo,Zou Yang,Sun Zhiyi,Hu Qiao,Chen Guokang,Chen Wenxing,Liu Xi,Zhong Ziyi,Xu Guangwen,Zhu Tingyu,Su Fabing
Developing high-performance Pt-based catalysts with low Pt loading is crucial but challenging for CO oxidation at temperatures below 100 °C. Herein, we report a Pt-based catalyst with only a 0.15 wt% Pt loading, which consists of Pt–Ti intermetallic single-atom alloy (ISAA) and Pt nanoparticles (NP) co-supported on a defective TiO 2 support, achieving a record high turnover frequency of 11.59 s –1 at 80 °C and complete conversion of CO at 120 °C. This is because the coexistence of Pt–Ti ISAA and Pt NP significantly alleviates the competitive adsorption of CO and O 2 , enhancing the activation of O 2 . Furthermore, Pt single atom sites are stabilized by Pt–Ti ISAA, resulting in distortion of the TiO 2 lattice within Pt–Ti ISAA. This distortion activates the neighboring surface lattice oxygen, allowing for the simultaneous occurrence of the Mars-van Krevelen and Langmuir–Hinshelwood reaction paths at low temperatures.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Pingzhen Li,Changlong Zheng,Zhen Zhang,Wei Liu,Xiaodong Wu,Shuang Liu
Due to the difficulty of integrating platinum into the perovskite lattice, it is yet challenging to build robust Pt catalysts through the “exsolution” strategy. In this article, we showed that by simply inserting a 500 ℃ holding period in the calcination process of a precursor that obtained via citric acid-assisted sol-gel methods, a homogeneous Pt-incorporated LaFeO 3 perovskite could be synthesized. Further characterizations evidenced that a La 4 PtO 7 phase, probably derived from the reactions among Pt ensembles, gaseous O 2 , crystallized La 2 O 2 CO 3 and La(OH) 3 , played a key role in preserving the platinum in a “dissolved” state during perovskite crystallization. Based on this perovskite system, an “intelligent catalyst” with well-dispersed exsolved Pt nanoparticles and relatively large surface area was produced, which was not only highly reactive for the complete oxidation of C 3 H 6 and CO, but also immune to the sintering effects induced by aging treatments. The above observations provide a typical example on how the slight changes in synthesis significantly influence the structure-property relationship of the catalysts obtained via exsolution methods, and how to utilize these knobs to obtain practical catalysts.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2024
·
IF 3.7
Zhengjian Hou,Yuanyuan Zhu,Hua Chi,Li Zhao,Huijie Wei,Yanyan Xi,Lishuang Ma,Xiang Feng,Xufeng Lin
Tuning Strong Metal-support Interactions (SMSI) is a key strategy to obtain highly active catalysts, but conventional methods usually enable TiO x encapsulation of noble metal components to minimize the exposure of noble metals. This study demonstrates a catalyst preparation method to modulate a weak encapsulation of Pt metal nanoparticles (NPs) with the supported TiO 2 , achieving the moderate suppression of SMSI effects. The introduction of silica inhibits this encapsulation, as reflected in the characterization results such as XPS and HRTEM, while the Ti4 + to Ti3 + conversion due to SMSI can still be found on the support surface. Furthermore, the hydrogenation of cinnamaldehyde (CAL) as a probe reaction revealed that once this encapsulation behavior was suppressed, the adsorption capacity of the catalyst for small molecules like H 2 and CO was enhanced, which thereby improved the catalytic activity and facilitated the hydrogenation of CAL. Meanwhile, the introduction of SiO 2 also changed the surface structure of the catalyst, which inhibited the occurrence of the acetal reaction and improved the conversion efficiency of C=O and C=C hydrogenation. Systematic manipulation of SMSI formation and its consequence on the performance in catalytic hydrogenation reactions are discussed.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Junjie Hao,Ning Li,Jingkai Lin,Chaorui Xue,Qing Chang,Xiangqian Fan,Huinian Zhang,Caihong Hao,Huayang Zhang,Shengliang Hu
Photocatalytic hydrogen production holds promise for solar energy conversion but is limited by inefficient charge separation and sluggish interfacial kinetics. Here, we construct a Pt@carbon nanotubes (CNTs)/ZnIn 2 S 4 (ZIS) heterostructure, where Pt-decorated CNTs intertwine and embed within ZIS microspheres. The CNTs not only guide ZIS nucleation but also serve as conductive channels and spatial confinement scaffolds, forming a well-integrated architecture for efficient carrier transport. This heterostructure operates via a thermo-electronic channel engineering strategy, integrating dual photothermal activation (arising from CNTs lattice vibrations and Pt plasmonic effects) with Schottky junction modulation. The resulting localized heating, in concert with the built-in electric field, synergistically enhances charge separation, facilitates hot electron generation, and accelerates interfacial reaction kinetics. The hierarchical architecture enables a three-dimensional hot-carrier migration pathway, efficiently directing electrons from the interior of ZIS to Pt active sites through CNTs. Consequently, the heterostructure achieves a hydrogen evolution rate of 51.4 mmol g −1 h −1 , 103 times higher than pristine ZIS. This work thus presents a multifunctional design paradigm that integrates efficient light harvesting, interfacial charge regulation, and thermal enhancement, providing a viable route toward highly efficient solar-driven hydrogen production.
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ACS Catalysis
·
2025
·
IF 13.1
Zhitong Zhou,Weixiang Guan,Xiaoli Pan,Aiqin Wang,Tao Zhang
One-pot amination coupling of vicinal diols toward the synthesis of pyrazines provides an efficient and economically viable route to access N-heterocycles from biomass, yet the current methodology relies on a fragile homogeneous catalyst system, which limits the sustainability of the chemistry. In this work, we developed a highly efficient heterogeneous catalyst 0.8Pt/13CeO2/Al2O3 which afforded diverse substituted pyrazines from readily available vicinal diols and ammonia with a yield up to 94% under mild reaction conditions and could be reused at least 6 times without obvious activity decay. Compared to the Pt/Al2O3 catalyst, the 0.8Pt/13CeO2/Al2O3 catalyst exhibited a 30-fold faster conversion rate of diols and an increased pyrazine selectivity from 48% to 79%. Characterizations revealed that doped CeO2 improved the dispersion of Pt, increased the electron density on the Pt sites, optimized the acid/basic property of the catalyst, and enhanced the adsorption strength and dehydrogenation ability of diols. All these features contributed to the increased activity and selectivity.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Fulin Yang,Wei Qiao,Lice Yu,Shuli Wang,Ligang Feng
Hydrogen generation from methanol via methanol-assisted water splitting is a promising electrochemical energy conversion technology but still meets challenges in addressing the low intrinsic activity and easy poisoning problems of the conventional Pt catalysts. Herein, the support engineering modulated Pt by hierarchical MoSe 2 @mesoporous hollow carbon support was proposed to integrate some structural and catalytic advantages for hydrogen evolution reaction (HER) and methanol oxidation reaction (MOR). Supporting engineering by layered MoSe 2 nanosheets confined in mesoporous hollow carbon spheres (MHCSs) is adopted to uniformly anchor Pt nanoparticles (Pt/MoSe 2 @MHCS), which effectively enhances the conductivity and prevents the layer-by-layer stacking of MoSe 2 ; Strong interaction and coupling ability between Pt and MoSe 2 and the resultant electronic structure regulation of the active centers could weaken the binding strength of CO* and H* intermediates during catalysis and strengthen the oxophilicity leading to improved MOR and HER kinetics. Specifically, Pt/MoSe 2 @MHCS shows a significantly improved MOR current density of 81.1 mA cm −2 , about 3.0 times that of the benchmark Pt/C catalyst. Meanwhile, it also exhibits the HER performance of 28 mV to achieve a kinetic current density of 10 mA cm −2 in methanol-contained electrolytes. When employed for overall methanol electrolysis, a lowered input voltage of 1.11 V can be obtained to drive the current density (10 mA cm −2 ) compared to that for water electrolysis (0.62 V vs. 1.73 V). The electrochemical properties of high activity, rapid catalytic kinetics, and good stability were also demonstrated due to the enhanced oxophilicity and high poisoning tolerance ability resulting from the MoSe 2 /carbon substrate-induced electron redistribution of Pt sites. This work reports a novel platform to address the catalysis challenges in hydrogen production via the methanol electrolysis technique.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yi Yao,Zixin Gao,Zhongjie Pan,Yanping Zhong,Lili Qin,Kexin Zhao,Shuhan Liu,Shengqing Zhang,Haoyang Han,Feiying Yin,Ruizheng Liang,Jinmin Zhao,Li Zheng
Platinum (Pt)-based nanozymes that effectively exert antioxidant effects exhibit great potential in the treatment of osteoarthritis (OA). However, these nanozymes are easy to agglomerate and have low catalytic efficiency, which can hardly meet the criterion of clinical therapy. To achieve efficient ROS removal, this study develops a novel ultrasound (US)-responsive piezoelectric nanozyme (MOF(Hf)-Pt) based on Pt with multi-enzyme mimicking activities and metal-organic frameworks (MOFs) with excellent piezoelectric properties. Results show that MOF(Hf)-Pt has excellent piezocatalytic enzyme activity, which can be adjusted by varying the intensity and time of US. Mechanistically, MOF(Hf)-Pt can increase ATP output and restore mitochondrial function, thereby reducing inflammatory factor levels. In vivo studies also reveal that under suitable US action, MOF(Hf)-Pt nanozymes can effectively inhibit the deterioration of OA, with reductions in OARSCI scores of 76.90 % and 82.66 % after 4 and 8 weeks, respectively. Particularly, the piezoelectric catalytic effect generated by MOF(Hf)-Pt can reverse oxidative stress-induced articular cartilage damage and promote cartilage regeneration, making it a promising candidate for OA treatment.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Chonghui Zhu,Yu Liang,Chenshuai Han,Zhaorui Zhang,Huashuai Hu,Minghui Yang
Efficient monitoring of hydrogen sulfide (H2S) in wastewater is essential for preventing environmental contamination and safeguarding public health. Current methods for assessing sulfide levels are limited by complex, time-consuming processes. Here, we introduce a Pt/CrWN2-based electrochemical gas sensor designed for real-time detection of H2S gas, offering a fast, reliable, and cost-effective solution for monitoring sulfate concentrations in wastewater. It exhibits rapid response and recovery times (3.6/3.5 s), high sensitivity (0.295 μA/ppm), and stability (90 days), even after direct exposure to sewage. Our findings demonstrate the potential of this system for continuous water quality assessment, providing valuable insights into pollution dynamics and enhancing environmental monitoring capabilities.
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