Catalysis Science & Technology
·
2018
·Vol. 8
·期 24
·6384-6395
·
IF 5.365
Zhiyang Zhang,Yanle Li,Jing Gu,Liping Ding,Nianhua Xue,Luming Peng,Xuefeng Guo,Yan Zhu,Jing Ma,Weiping Ding
The electrostatic field of a dielectric cavity is powerful for modulating many aspects of confined metal clusters. Here we report that the catalytic properties of Ptn clusters confined in X-zeolite cages are strongly tuned by altering the zeolitic field, which is achieved by using different cations (Na+, Cs+, Ca2+ or La3+) to balance the negative framework of the zeolite. Compared with Ptn@LaX, for example, Ptn@CsX shows a surprising ∼5500% enhancement in TOF value for phenol hydrogenation to cyclohexanol. Electrostatic field modulation leads to gradual changes of electronic properties such as the Fermi levels/d-band centers of the Ptn clusters, as revealed by DFT calculations and experimental characterizations. The decreases in Fermi levels of the Ptn clusters benefit the hydrogenation of –CCH groups (phenylacetylene and acetylene) and –NO2 groups (nitrobenzene, o-nitroanisole and o-chloronitrobenzene) but are detrimental for aromatic ring hydrogenation (phenol). These findings are important for the design of high performance catalysts.
研究领域:
化学
·
材料科学
✓ 已验证
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 26
·期 4
·3263-3273
·
IF 3.3
Ziwei Zhai,Bofeng Zhang,Yutong Wang,Guozhu Liu
Based on the disturbance of electronic density, nitrogen-doped nanocarbons show promising properties to anchor metal clusters. However, precisely regulating the coordination mode between N species and the active site remains challenging. Herein, we rationally designed three N types (graphitic N, pyridinic N and pyrrolic N) in nanocarbons to anchor Pt clusters for the benchmark propane dehydrogenation. The specific activity of the pyridinic-N-doped catalyst was 147.54 molC3H6 molPt−1 h−1 at 550 °C, which was 1.3 times higher than those of graphitic- and pyrrolic-N-doped catalysts. Unlike the regular tetrahedron Pt cluster in the graphitic-N catalyst or the distorted three-layered Pt cluster in the pyrrolic-N catalyst, the Pt cluster in the pyridinic-N catalyst was an inverted tetrahedron, which increased the contact degree without geometric repulsion towards C–H bond scission. The geometric parameters of detached H and C atoms in the methylene group for the pyridinic N catalyst was decreased to strengthen the C–H bond scission. After CH3CHCH3* adsorption, the Bader charge of the Pt active site also became highly positive, which tailored the d-band center closer to the Fermi level and provided more vacant orbitals for C–H bond breakage. Therefore, pyridinic N in nanocarbons is promising to anchor small-sized Pt for alkane dehydrogenation in terms of geometric and electronic effects.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2019
·
IF 12.221
Jiayun Zhang,Yuchen Deng,Xiangbin Cai,Yunlei Chen,Mi Peng,Zhimin Jia,Zheng Jiang,Pengju Ren,Siyu Yao,Jinglin Xie,Dequan Xiao,Xiaodong Wen,Ning Wang,Hongyang Liu,Ding Ma
Tin-assisted fully exposed Pt clusters are fabricated on the core–shell nanodiamond@graphene (ND@G) hybrid support (a-PtSn/ND@G). The obtained atomically dispersed Pt clusters, with an average Pt atom number of 3, were anchored over the ND@G support by the assistance of Sn atoms as a partition agent and through the Pt–C bond between Pt clusters and defect-rich graphene nanoshell. The atomically dispersed Pt clusters guaranteed a full metal availability to the reactants, a high thermal stability, and an optimized adsorption/desorption behavior. It inhibits the side reactions and enhances catalytic performance in direct dehydrogenation of n-butane at a low temperature of 450 °C, leading to >98% selectivity toward olefin products, and the turnover frequency (TOF) of a-PtSn/ND@G is ∼3.9 times higher than that of the traditional Pt3Sn alloy catalyst supported on Al2O3 (Pt3Sn/Al2O3).
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Pai Peng,Yaning Yue,Mengxi Han,Jun Shi,Jing Yang,Junwen Chen,Qiang Chen
Design of heterogeneous catalyst to achieve efficient conversion of biomass to high added-value chemicals is still very attractive. Herein, taking industrially important selective hydrogenation of furfural to furfuryl alcohol as an example, the designed amorphized HA zeolite encapsulation of platinum clusters (denoted as Pt@HA) exhibited excellent catalytic selectivity at totally conversion of the reactant furfural, along with good reusability and poison resistance ability. The selected amorphized HA zeolite with very small pore size constrained the reactant furfural to be reacted through hydrogen spillover process at zeolite surface, instead of to be adsorbed and activated onto Pt surface. Resulting from the stronger interaction between nucleophilic oxygen atom of aldehyde group and acid site at HA zeolite surface than that of furan ring group, furfural preferred to adsorb onto Pt@HA surface with the end of aldehyde group rather than the end of furan ring group, thus facilitating the spilled H atom to react with aldehyde group to give desired furfuryl alcohol product exclusively.
研究领域:
催化化学
·
生物质转化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Shuwen Jin,Guangyao Zhang,Zhanyue Huo,Libei Feng,Mengyi Liu,Zhiyuan Sun,Diab Khalafallah,Jue Wang,Qinfang Zhang
Hydrogen energy, as a clean and renewable alternative to fossil fuels, requires efficient electrocatalysts for sustainable hydrogen production via the hydrogen evolution reaction (HER). Platinum-based catalysts exhibit superior HER activity but face challenges of high cost, instability, and aggregation under acidic conditions. MXenes, two-dimensional materials with high conductivity and tunable surface chemistry, offer promising support platforms to enhance platinum utilization. Here, we report the design of highly active and stable HER catalysts by anchoring sub-nanometer platinum clusters onto lamellar Ti 3 C 2 and Nb 2 C MXenes via a cluster beam deposition technique. The optimized Pt/Ti 3 C 2 catalyst achieves a low overpotential of 67 mV at 10 mA cm −2 in acidic media, outperforming Pt/Nb 2 C (72 mV), pure Pt clusters (79 mV), and commercial Pt/C (82 mV). This enhancement arises from Ti 3 C 2 's larger surface area, which stabilizes Pt clusters, prevents aggregation, and facilitates interfacial electron transfer. The Pt/Ti 3 C 2 heterojunction also demonstrates a Tafel slope of 26.3 mV dec −1 , indicating rapid Volmer-Tafel kinetics, and retains 95 % activity after 5 h of operation. Compared to prior Pt/MXene systems, this work highlights the critical role of MXene surface functionality and Pt cluster dispersion in optimizing HER performance. By reducing platinum loading while maintaining high efficiency, this strategy advances the development of cost-effective electrocatalysts for scalable green hydrogen production. Our findings provide a blueprint for engineering MXene-supported metal clusters to address energy and sustainability challenges.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Jianfeng Li,Shenglong Ding,Fushan Wang,Huacheng Zhao,Jinfang Kou,Muhammad Akram,Manhua Xu,Wu Gao,Chuang Liu,Huangruoyin Yang,Zhengping Dong
Chemoselective hydrogenation of unsaturated organic compounds is a significant research topic in the catalysis field. Herein, a sulfur-doped ordered mesoporous carbon (SMC) material was prepared to anchor ultrafine platinum (Pt) clusters for the chemoselective hydrogenation of halogenated nitroarenes. The confinement effect of the ordered pores and the strong metal-support interaction caused by Pt clusters and sulfur atoms, efficiently suppress the aggregation and regulate the electronic states of the ultrafine Pt clusters. Thus, the hydrogenation of parachloronitrobenzene ( p -CNB) shows high selectivity catalyzed by the ultrafine Pt clusters with electron-rich states. Meanwhile, the catalytic performance of the hydrogenation reaction catalyzed by Pt/SMC is capable of being maintained after at least 5 cycles, and the catalytic universality can also be applied to different halogenated nitroarenes hydrogenation. Therefore, this study may promote the research into the construction of noble metal-based catalysts for chemoselective hydrogenation reactions in green and sustainable chemical processes.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Xin Sun,Jing Yu,Yan Zhang,Qi Liu,Rongrong Chen,Jingyuan Liu,Jiahui Zhu,Jun Wang
Atomic clusters exhibit superior performance in heterogeneous catalysis due to their unique electronic states and highly exposed active surfaces. Nevertheless, significant challenges persist in achieving the precise and efficient synthesis of atomic clusters while preventing undesirable formation of coexisting species, particularly nanoparticles. Herein, a one-step in situ phase transition engineering strategy is reported for the synthesis of atomic platinum clusters by vapor deposition on Ti 3 C 2 Cl 2 MXene and TiC heterogeneous interface (Pt-MXene/TiC) in molten salt, where Pt clusters can be acquired over a slight amount of Pt contents (0.298 wt.%). The strongly polarized molten salt induces the desired confinement of atomic-scale Pt clusters. The construction of heterogeneous interfaces enhances the local electric field and accelerates the electron transfer between Pt and the substrate. As a result, Pt-MXene/TiC-950 exhibits an exceptional increase in mass activity and turnover frequency (TOF) for hydrogen evolution reaction (HER) at 49.4 and 46.7 folds of 10% commercial Pt/C. Further theoretical calculations elucidate that the Pt species in Pt-MXene/TiC-950 possess moderate d-band center, which enables optimized selectivity and activity for intermediates adsorption in HER process. This work provides some guidelines for leveraging molten salt and heterostructure to enhance the precision and synthesis efficiency of atomic clusters.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Hao Liu,Ying Zhang,Liyang Liu,Tianxiang Chen,Xingcong Zhang,Peng Hu,Chao Xiong,Jie Zhou,Hao Zhang,Lihui Dong,Tsz Woon Benedict Lo,Bing Nan,Xiaohui He,Hongbing Ji
Dispersing metals from nanoparticles to clusters is often achieved using ligand protection methods, which exhibit unique properties such as suppressing structure-sensitive side reactions. However, this method is limited by the use of different metal precursor salts corresponding to different ligands. An alternative approach, the ion exchange (IE) method, can overcome this limitation to some extent. Nevertheless, there is still an urgent need to address the stabilization of metals (especially precious metals) by using IE method. Here, we reported a Pt cluster catalyst prepared mainly by anchoring Pt atoms via O located near the framework Zn in zincosilicate zeolites and riveted by zeolite surface rings after reduction (reduced Pt/Zn-3-IE). The catalyst can achieve an initial propane conversion of 26% in a pure propane atmosphere at 550 °C and shows little deactivation even after 7.5 d of operation. Moreover, the alteration of catalyst by the introduction of framework Zn was also highlighted and interpreted.
研究领域:
催化
·
材料科学
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Chao Wang,Hu Zang,Changjiang Liu,Jiahao Wang,Long Kuai,Baoyou Geng
The hydrogen evolution reaction (HER) involves two-step elementary reactions, providing an opportunity to establish dual-site synergistic catalysts. This work demonstrates carbon-supported Pt single atoms and clusters (Pt1+Cs-NPC) as an efficient catalyst for acidic HER, which exhibits an ultralow Tafel slope of 12.5 mV/dec and an overpotential of 24 mV at 10 mA/cm2 with an ultralow platinum content of 3.8 wt %. The Pt mass activity and turnover frequency (TOF) are 10.2 times and 5.4 times that of commercial Pt/C, respectively. The density functional theory (DFT) study shows that the Pt cluster regulates the electronic state structure of the adjacent Pt single atom, so that the ΔGH* at the Pt1 site approaches 0. Moreover, the DFT study confirms that Pt clusters and neighboring Pt single atoms can synergistically catalyze the Tafel step and reduce the energy barrier in forming the H–H bond. At the same time, the platinum cluster reduces the energy barrier of the nearby platinum single-atom site to the Heyrovsky step and accelerates the reaction with hydrated hydrogen ions. Studies have shown that platinum clusters and platinum single-atom composite loading structures exhibit excellent activity for the Volmer–Tafel or Volmer–Heyrovsky reaction paths of HER reactions. This work provides a clear understanding of the synergistic effect of Pt1+Cs-NPC, which provides guidance for developing efficient HER catalysts.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2021
·
IF 9.676
Yihan Feng,Zichuang Li,Shanlin Li,Minghui Yang,Ruguang Ma,Jiacheng Wang
Integrating active Pt clusters into transition-metal oxides with water-dissociation ability is effective to prepare a bifunctional electrocatalyst for water splitting in alkaline. However, the additional utilization of a reductant and/or the operation at the elevating temperature causes the over-growth and agglomeration of Pt clusters, thus losing the high catalytic performance. Herein, we report that V dopant not only favors self-reducing Pt clusters on NiFe layered double hydroxide (LDH) (Pt/NiFeV) at room temperature, but also regulates interfacial charge redistribution to enhance the water-splitting performance. Experimental and theoretical studies reveal that V dopant into NiFe LDH triggers more electrons to transfer to adjacent Fe atoms, thus leading to a higher reducing ability compared to that without V-doping. When used as water-splitting electrocatalyst, V doping promotes electron loss of Pt clusters in Pt/NiFeV, optimizing the free energy of hydrogen adsorption and proton recombination kinetics at the cathode. Meanwhile, it also moves the d-band center of Ni away from the Fermi level to optimize the adsorption of *OH intermediates and facilitate the desorption of oxygen molecules at the anode. Thereby, Pt/NiFeV exhibits much higher bifunctional performance than V-free Pt/NiFe LDH toward both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). This work can spark inspiration of designing other bifunctional electrocatalysts for energy conversion and storage.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Songjie Li,Tiantian Liu,Shuang Yu,Xiaomei Yu,Huijing Yang,Chengduo Wang,Jin You Zheng
Hydrogen production via electrocatalytic water splitting has garnered significant attention, due to the growing demand for clean and renewable energy. However, achieving low overpotential and long-term stability of water splitting catalysts at high current densities remains a major challenge. Herein, a CoP@CoNi layered double hydroxide (LDH) electrode was synthesized via a two-step electrodeposition process, demonstrating oxygen evolution reaction, with an overpotential (ƞ 400 ) of 373 mV and a Tafel slope of 64.2 mV/dec. Subsequently, a superhydrophilic CoP@CoNi LDH-Pt electrode was prepared using an in situ oxidation method, with Pt clusters anchored within the CoP@CoNi LDH for the hydrogen evolution reaction, with an overpotential (ƞ 400 ) of 119 mV and a Tafel slope of 33.6 mV/dec. The CoP@CoNi LDH-Pt||CoP@CoNi LDH system achieved a cell voltage of 1.96 V at 1000 mA/cm 2 , maintaining stable performance after water electrolysis for 160 h. These remarkable outcomes stem from the fast charge transfer, improved mass transfer, and superior stability of the catalysts. Heterostructure electrodes were constructed to optimize the electrocatalytic kinetics through strong interfacial electronic interactions, while superhydrophilic electrodes were fabricated to improve the mass transfer process at a high current density. Anchoring high-activity components in catalysts prevents their detachment during water electrolysis, enhancing the structural stability of the electrodes. This study provides a new approach for large-scale preparation of efficient water electrolysis catalysts and offers significant potential for industrial hydrogen production applications.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small Methods
·
2019
·Vol. 3
·期 5
·1800510
·
IF 0
Dongxu Wang,Jiancong Liu,Xusheng Cheng,Xin Kang,Aiping Wu,Chungui Tian,Honggang Fu
The significant increase of catalytic efficiency while remaining low Pt usage is constantly pursued, but remains a challenge. Here, a “vacuum-assisted” (VA) process toward Pt clusters dispersed on SAPO-11 (S-11) is shown for a high-effective hydroisomerization of n -C 16 . The VA can make effective trapping of the Pt precursor on S-11 due to intensive capillary action, being conductive to stabilize and disperse Pt cluster (≈1 nm) on S-11 (V-Pt/S-11) for promoting synergy of Pt sites and acid sites on S-11. The test indicates excellent catalytic activity and stability of trace Pt clusters (0.15 wt%, even lower, 0.035 wt%) on S-11 (≈94.4% isomer selectivity at 94.3% conversion), much superior to I-0.15 wt% Pt/S-11 from traditional impregnation routes (≈88% selectivity at 90% conversion) and ever reported catalysts. The V-Pt/S-11 is also superior for the hydroisomerization of catalytic diesel oil with a decrease of freezing point up to 40 °C after hydroisomerization. The superior performance is attributed to the exposure of high acid density due to little coverage of Pt cluster on S-11, high dispersion of Pt leading to form more metal–acid bifunctional sites, and enhanced (de)hydrogenation ability of Pt clusters. All of them can promote the effective synergy of metal sites (Pt) and acid sites.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
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