CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Yirui Jiang,Jianfang Liu,Hongru Liu,Yong Wang,Yongzhi Zhao,Sijia Liu,Yunpu Qin,Zihao Li,Hong Zhao,Hao Li,Haoyang Wu,Deyin Zhang,Luan Liu,Baorui Jia,Xuanhui Qu,Mingli Qin
Platinum (Pt) metal is widely acknowledged as a highly efficient electrocatalyst for hydrogen evolution reaction (HER) in acidic electrolyte. However, its performance in alkaline environments is significantly lower owing to the sluggish water dissociation step. Herein, we synthesized an ultrahigh Pt-mass-activity alkaline HER catalyst using microwave reduction method in air. Our catalyst, PtRu@CNT, comprises PtRu alloy nanoparticles uniformly loaded on carbon nanotubes, with Pt and Ru contents of 12.3 wt% and 4.5 wt%, respectively. The PtRu alloy nanoparticles have an average diameter of about 3 nm and a face-centered cubic structure, and the introduction of Ru has led to a modified electronic structure in Pt. As a result, an impressively low HER overpotential of 13 mV was achieved, significantly lower than commercial 20 wt% Pt/C (61 mV). PtRu@CNT exhibited a high turnover frequency based on metal mass of 3.06 s −1 at 100 mV, about 6 times higher than commercial Pt/C (0.46 s −1 at 100 mV), highlighting its excellent intrinsic activity. The HER mechanism of PtRu@CNT is a Volmer-Tafel mechanism, where the rate-limiting step changed to the recombination of hydrogen atoms from initial water dissociation, attributed to the presence of Ru. The alkaline HER activity of PtRu@CNT ranks among the best of currently reported Pt-based catalysts.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Meichun Fu,Zhiyu Shao,Yuan Zhang,Qian Zhu,Kuo He,Mengzhu Zhang,Yuzhu Hou,Laiping Fang,Fei Yan,Shuang Zhang,Jianshi Du,Ping’an Ma,Keke Huang,Shouhua Feng
Despite the multiple advantages of high tissue penetration depth, selectivity, and noninvasiveness of photothermal-assisted antitumor synergistic therapy, developing photothermal agents with multifunctional characteristics, desirable tumor therapeutic effects, and biological stability remains a key challenge. Herein, an electronic structure-regulated strategy is proposed to activate self-adaptive Sn–Fe electron pair centers (Sn2+/Sn4+ and Fe2+/Fe3+) through loading the electron donor Pt (Pt/SFO-1, -2, -3, -4). Experimental and theoretical calculations indicate that abundant dynamic active centers can facilitate the production of reactive oxygen species (ROS), which enables Pt/SFO samples to possess catalase (CAT), peroxidase (POD), and oxidase (OXD) enzyme-like activities. Upon near-infrared (NIR) laser irradiation, Pt/SFO-2 with a Pt load of 0.9% achieves the highest ROS production, showing a 9-fold compared with SnFe2O4 and implements the synergistic therapy of photothermal therapy (PTT), photodynamic therapy (PDT), and chemodynamic therapy (CDT). The electronic state regulation of inorganic photothermal agents not only improves tumor therapeutic effects but also offers a novel strategy to regulate the electron structure of active centers.
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Materials Today Chemistry
·
2025
·
IF 6.7
Chen Shen,Haiyong Wang,Tianyu Ren,Tianhan Zhu,Tianyu Gao,Mi Luo,Xiaoman Wang,Tong Zhang,Chenguang Wang
The cascade amination of nitrobenzene with benzaldehyde represents an environmentally benign route for imine synthesis in fine chemistry. Nevertheless, challenges including harsh reaction conditions, inefficiency, and poor selectivity hinder its practical implementation. Herein, we report a Pt/Zn x Fe 3-x O y interfacial catalyst system that synergistically modulates both electronic states of Pt nanoparticles (NPs) and acid/base properties of the support to address these limitations. Controlling of chemical composition of Zn x Fe 3-x O y to can efficient regulate electronic state of Pt and acid/base sites of Pt/Zn x Fe 3-x O y . The catalytic performance was strongly dependent on the interfacial electronic interactions and acid-base properties at the Pt/Zn x Fe 3-x O 4 interface. Due to lower work function of ZnFe 2 O 4 , interfacial electrons transfer to Pt from ZnFe 2 O 4 support form rich-electronic Pt accelerated hydrogenation of nitrobenzene. Rich oxygen vacancies and hydroxyl groups as acid and base sites, optimize condensation efficiency and intermediate desorption. This dual regulation strategy achieves exceptional catalytic performance under mild conditions (30 °C, 1 MPa H 2 , 4 h), delivering 96.0 % conversion with 96.25 % imine selectivity. More than 20 different amines compounds and gram-scale of imines (1.495 g) were synthesized over Pt/ZnFe 2 O 4 . In-situ DRIFTS spectroscopy identifies aniline as the critical intermediate, confirming the proposed cascade mechanism. Our work establishes a materials design paradigm leveraging support composition to reconcile electronic and acid-base requirements in tandem catalysis.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Liwu Qiang,Xuemin Yang,He Xiao,Peipei Zhao,Qinyun Yan,Wei Wen,Chunmei Liu,Qilin Guo,Yanxia Zhang,Man Zhao,Jianfeng Jia
Electrolytic water splitting for hydrogen production is considered as one of the promising directions due to its environmental friendliness and high generated hydrogen purity. To address the high overpotential caused by the sluggish kinetics of the oxygen evolution reaction (OER), a modified four-electrode system has been designed to synthesize bifunctional PtCo/graphene (PtCo/G) composites, which feature dual active sites. This method allows for the electrolysis of Pt at a high voltage (30 V) and Co at a lower voltage (10 V), while graphene is prepared through the exfoliation of graphite sheets at the cathode. This process concurrently resolves the issues of differential dissolution voltages between Pt and Co and the poor conductivity of the material, achieving the efficient synthesis of metal/graphene composites. The PtCo/G-2h composite exhibits excellent electrocatalytic activity. In the 0.5 M H 2 SO 4 , the overpotential for hydrogen evolution reaction (HER) at 10 mA cm −2 is 18 mV lower than that of commercial Pt/C catalyst. In 1 M KOH, PtCo/G-2h demonstrates superior electrocatalytic OER activity, with an overpotential at 10 mA cm −2 that is only 2 mV higher than that of the commercial RuO 2 catalyst. As a bifunctional catalyst for water electrolysis, the PtCo/G composites can effectively facilitate the adsorption of OH − ions, and assist in altering the rate-determining step, thus significantly reducing the activation energy (E a ) of the reaction. This work introduces a novel approach for the synthesis of graphene-based materials using a self-designed electrochemical method.
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Journal of Environmental Sciences
·
2025
·
IF 6.3
Rongrong Hong,Yunshuo Wu,Yuetan Su,Chu Qin,Haiqiang Wang,Xuanhao Wu,Zhongbiao Wu,Xiaole Weng
Highly efficient catalysts for methane combustion have long been pursued due to the intrinsic inertness of CH 4 . In this work, bimetallic PtIr/TiO 2 catalysts with varying Pt:Ir ratios were synthesized to modulate the electronic structures of the metals, thereby achieving bimetallic synergy to enhance CH 4 combustion activity. Among the series of monometallic and bimetallic catalysts, Pt 0.5 Ir 0.5 /TiO 2 exhibited the highest activity, achieving complete CH 4 conversion (T 100 ) at 370°C after activation during the first reaction cycle. Combined experimental and computational studies elucidated that the incorporation of Ir facilitated electron transfer and the formation of partially oxidized Pt δ+ (0 < δ < 2) species, which were coordinatively unsaturated and more conducive for CH 4 oxidation. The high affinity of Ir for oxygen enabled the Pt δ+ species to be stabilized under CH 4 oxidation reaction conditions, instead of being overoxidized into Pt 2+ species as in the monometallic Pt 1 /TiO 2 catalyst. Simultaneously, Ir species in the bimetallic catalyst were oxidized into Ir δ+ species during the reaction and ultimately formed the Pt δ+ -O-Ir δ+ interface to further elevate the reaction activity. Moreover, the bimetallic catalysts integrated the merits of Ir for CH 4 adsorption and Pt for intermediates conversion, synergistically boosting the reaction activity. This work provides insight into designing effective CH 4 combustion catalysts through fine-tuning the metal electronic structures.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Xining Guo,Huiying Li,Leshi Zhang,Rui Hao,Fei Ye,Jianmin Gu,Kaihang Sun,Guozhu Li,Ji−Jun Zou,Zhourong Xiao,Desong Wang
The photothermal catalytic conversion of CO2 into value-added chemicals is of great significance for realizing the goal of carbon neutralization. However, these catalysts have problems such as an insignificant photothermal effect and high recombination of photogenerated carriers. Here, porous TiO2 was prepared by hydrothermal crystallization and topological conversion of metal–organic frameworks (MOFs), and loaded with highly dispersed Pt catalysts to realize an efficient photothermal catalytic reverse water-gas shift (RWGS) reaction. N2-adsorption results showed that the as-prepared Pt/TiO2 catalysts had an abundant mesoporous structure, thus contributing to the rapid diffusion of reactants and light transport. X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) results showed that Pt was uniformly dispersed on the catalyst surface with an average particle size of 2.06 nm. H2-TPR profiles showed that the Pt/TiO2 catalyst had strong metal–support interactions, CO2-TPD showed its strong CO2 adsorption capacity, and CO-TPD showed its weak CO adsorption strength. In situ X-ray photoelectron spectroscopy (XPS) showed that the electron cloud density on the Pt surface further increased under light illumination, which contributed to the activation and dissociation of H2. In addition, the Pt/TiO2 catalyst had a narrow band gap width and sufficiently low reduction potential, and its excellent photothermal and photovoltaic properties ensured efficient performance in the photothermal RWGS reaction. The Pt/TiO2 catalysts showed a high CO2 conversion of 29.8%, a product CO selectivity higher than 99.6%, and a stability of more than 3000 min at 350 °C, with a light intensity of 1.2 W cm–2 and a GHSV of 36,000 mL gcat–1 h–1.
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CATALYSIS LETTERS
·
2024
·
IF 2.3
Xu Xian,Lan Ling,Xu Jiangong,Liang Zheng,Tan Jin,Wang Haiyong,Qiu Songbai
The development of biodegradable materials from biomass is a crucial strategy for leveraging biomass resources. A key component in this process is 2,5-bis(hydroxymethyl)furan (BHMF), a significant biomass-derived platform chemical. However, producing BHMF with high selectivity through the selective hydrogenation of 5-hydroxymethylfurfural, while avoiding the creation of unwanted byproducts, is a complex challenge. In our research, we have developed a novel catalyst featuring a magnetic core. This catalyst, which consists of platinum loaded onto a graphene-like shell, has been applied to the catalytic hydrogenation of HMF in an aqueous environment. Under the optimized conditions of 373 K, 3 MPa H 2 , and 1 h reaction time, a BHMF yield exceeding 99% was achieved. This method presents a promising and effective approach for the high-value conversion of biomass waste into polymer materials and pharmaceutical chemicals. Graphical Abstract
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Zhenze Xie,Yucheng Huang,Jingguang Wang,Wenxin Guo,Yutao Lin,Yingxin Lin,Chang Du
Breast cancer is one of the most widespread cancers worldwide in the female population. However, the side effects and toxicity of chemotherapy and radiotherapy are the obstacles to the treatment of breast cancer. Therefore, we developed a Pt loaded CoFe 2 O 4 -based nanoparticles (CF@Pt) for breast cancer treatment with chemodynamic therapy (CDT) and sonodynamic therapy (SDT). The Co 2+ /Co 3+ and Fe 2+ /Fe 3+ gave CF@Pt peroxidase-like activity and catalase activity to gain ·OH and O 2 in the tumor microenvironment (TME) for CDT. Furthermore, the separation of electron-hole pairs of CF@Pt transferred the O 2 into 1 O 2 in the presence of ultrasound (US) for SDT. The high level of O 2 generated by CDT would produce more 1 O 2 by SDT that promoted the CDT efficiency. Moreover, the addition of Pt limited the recombination of electron-hole pairs and reduced the energy gap to enhance SDT/CDT combination therapy. In addition, CF@Pt could be engulfed by MDA-MB-231 cells and induced the apoptosis while it had good biocompatibility and blood compatibility. This design provided a novel application on the treatment of breast cancer.
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MOLECULES
·
2025
·Vol. 30
·期 1
·187
·
IF 4.6
Shuqi Liao,Weisen Deng,Feng Yang,Jutao Zhou,Ling Wu,Donghong Yu,Zhong Cao
Compared to natural enzymes, the development of efficient artificial simulated enzymes, such as those based on bimetallic materials with high catalytic activity and good stability, is an important way until now. Herein, we employed ZnCo2O4microspheres as carriers to synthesize Pt-doped composites with different amounts using a one-pot method. The morphology and structure of the synthesized materials were characterized using XRD, SEM, BET, FT-IR, XPS, and Zeta potential techniques. It was found that Pt0adhered well to the surface of ZnCo2O4microspheres, with a 12.5% Pt doped ratio exhibiting abundant oxygen vacancies, excellent substrate affinity, and high peroxidase-like activity. Using fluorescent probes and electrochemical methods, the peroxidase-like catalytic mechanism has been explored that Pt@ZnCo2O4microspheres can accelerate the electron transfer between H2O2and 3,3′,5,5′-tetramethylbenzidine (TMB). Based on the optimal loading ratio of 12.5% of Pt@ZnCo2O4, a colorimetric sensor for visual detection of L-cysteine (L-Cys) was constructed, exhibiting a wide linear range of 0.1~50 µM and a low detection limit of 0.0163 µM. The sensor possesses good selectivity, reusability, and usage stability, which can be well applied to the determination of L-Cys in health product capsules with recovery rates of 96.9%~103.7% and RSD of 1.07%~6.50%. This work broadens the application prospects of spinel materials such as ZnCo2O4in the field of biological analysis and also provides inspiration for the development of new artificial simulated enzymes.
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ANALYTICA CHIMICA ACTA
·
2024
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IF 5.7
Meiling Chen,Yang Yang,Qinhua Chen,Lina Tang,Junlin Liu,Yujie Sun,Qiming Liu,Yulin Zhang,Guo-jun Zhang,Shaowei Chen
Cholesterol is an important lipid compound found in a variety of foods, and its level in human blood is closely related to human health. Therefore, development of rapid and accurate POCT (point-of-care testing) methods for cholesterol detection is crucial for assessing food quality and early diagnosis of diseases, in particular, in a resource-limited environment. In this study, a smartphone-assisted colorimetric biosensor is constructed based on platinum,phosphorus-codoped carbon nitride (PtCNP 2 ) for the rapid detection of cholesterol. Phosphorus-doped carbon nitride is prepared by thermal annealing of urea and NH 4 PF 6 , into which platinum is atomically dispersed by thermal refluxing. The obtained PtCNP 2 exhibits an excellent peroxidase-like activity under physiological pH, whereby colorless o -phenylenediamine (OPD) is oxidized to colored 2,3-diaminophenazine (DAP) in the presence of hydrogen peroxide (H 2 O 2 ), which can be produced during the oxidation of cholesterol by cholesterol oxidase. A smartphone-assisted visual sensing system is then constructed based on the color recognition software, and rapid on-site detection of cholesterol is achieved by reading the RGB values. Meanwhile, the generated DAP shows an apparent fluorescence signal and can realize highly sensitive detection of cholesterol by the change of the fluorescence signal intensity. Such a cholesterol sensor exhibits a wide linear detection range of 0.5–600 μg mL −1 and a low detection limit of 59 ng mL −1 . The practicality of the sensor is successfully demonstrated in the rapid detection of cholesterol in serum and food.
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ACS Catalysis
·
2025
·
IF 13.1
Yuanjing Zhang,Guanyi Zhang,Quandong Hou,Shiquan Zhao,Si Wang,Enze Xu,Lei Wang,Xin Zhang,Feng Li,Yusen Yang,Min Wei
Aqueous-phase tandem reactions, as a fundamental aspect of green chemistry, hold a crucial position in the contemporary synthesis of fine chemicals, wherein the advancement of high-performance heterogeneous catalysts remains a formidable challenge. Herein, we report a Pt1Con single-atom alloy (SAA) catalyst in which Pt single atoms are immobilized onto the surface of Co nanoparticles through Pt–Co coordination. The Pt1Con SAA catalyst exhibits a high chemoselectivity for the aqueous-phase hydrogenation–rearrangement reaction of furfural (FAL) to cyclopentanol (CPL) (yield: >93%, considering the carbon loss), with a TOF value of 2257 h–1 (based on Pt). A joint investigation based on reaction dynamics, isotope-label tracing experiments, EPR, and in situ FT-IR verifies a five-step consecutive tandem reaction pathway for the formation of CPL. Notably, during the reaction, the rapid exchange of hydrogen atoms would occur between activated hydrogen species and the water solvent. Furthermore, the water molecule does not serve as a H-donor but is involved in the rearrangement reaction in the side chain of the furan ring. Kinetic studies combined with DFT calculations substantiate that the Pt–Co interface sites effectively lower the energy barrier of the cyclopentanone (CPO) hydrogenation step via facilitating activation adsorption of the carbonyl group, accounting for the largely enhanced catalytic behavior. This study sheds light on the advancement of a highly efficient and stable heterogeneous catalyst for a biomass upgrading reaction in the aqueous phase.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Mengyin Liao,Chao Wang,Xuanhua Zhang,Chao Luan,Wenyuan Xu,Zhongyi He
Novel Pt/Co(OH)2-NiO/C catalysts based on carbon black were successfully synthesized using the hydrazine hydrate reduction method and galvanic replacement strategies. They were subsequently tested for their activity in the electrocatalytic oxidation of methanol. It was observed that the peak current density of Pt/Co(OH)2-NiO/C (8.29 A mg-1Pt) was 22.4 times higher than that of commercial Pt/C-JM (0.37 A mg-1Pt). The electrocatalytic activities and durabilities of the synchronously synthesized Pt/Co(OH)2-NiO/C catalysts were significantly better than those of PtCo/C, PtNi/C, and PtCoNi/C-X (X = 200, 400, 600) catalysts synthesized by calcination in Ar at different temperatures. The reason is that the highly dispersed Pt helps to expose more active sites on the catalyst surface, and the addition of Co(OH)2 and NiO alters the electron density of Pt, which reduces the adsorption of intermediate CO, attenuates the toxic effect, and enables more efficient oxidation of methanol.
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