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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 · IF 4.939

Enhancing selectivity and reducing cost for dehydrogenation of dodecahydro-N-ethylcarbazole by supporting platinum on titanium dioxide

Xiang Gong,Zhao Jiang,Tao Fang

N-ethylcarbazole/dodecahydro-N-ethylcarbazole (NECZ/12H-NECZ) was a promising system for hydrogen storage applications. 1.0 wt% Pt/TiO 2 was regarded as the optimal loading in Pt/TiO 2 catalyst applied in the 12H-NECZ dehydrogenation reaction. The hydrogen release amount, selectivity to NECZ and TOF of 12H-NECZ dehydrogenation are 5.75 wt %, 98% and 229.73 min −1 at 453 K. Compared with the commercial 5.0 wt% Pd and Pt-based catalysts, it exhibited very high activity, selectivity and stability for 12H-NECZ dehydrogenation with low Pt loading. Combined with the XRD , XPS , HRTEM , TPR analysis, it was indicated that the enhanced catalytic performance was due to the SMSI (strong metal-supporting interaction) between Pt and TiO 2 support, which accelerated the rate-limiting step and enhanced the whole dehydrogenation reaction. This work may be beneficial for the commercial application of Pt/TiO 2 catalysts in the Liquid Organic Hydrogen Carrier (LOHC) system.

研究领域: 化学工程 · 材料科学
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ENERGY & FUELS · 2021 · IF 3.605

Decarboxylation of Oleic Acid Using Pt@SAPO-11 Catalysts Fabricated by In Situ Encapsulation

Meiqiu Hu,Xiaolong Liu,Hong Yuan,Jingye Ma

An in situ encapsulation process was used to prepare ordered worm-like mesoporous Pt@SAPO-11 catalysts with different Pt loadings. Transmission electron microscopy images showed that Pt nanoparticles encapsulated within the SAPO-11 support mesopores were uniformly distributed and highly dispersed and had a narrow particle size distribution of 2–7 nm. Scanning electron microscopy indicated that increasing the Pt loading from 0.6 to 1.6 wt % did not significantly change the crystalline morphology of the catalyst, although the crystallinity decreased slightly. The specific surface area and average pore diameter of the Pt@SAPO-11 were in the ranges of 72–116 m2/g and 8.1–9.5 nm, respectively, which are determined by the Brunauer–Emmett–Teller method and Barrett–Joyner–Halenda method, respectively. The NH3 thermal-programmed desorption established that increasing the Pt loading gradually decreased the total NH3 desorption and that a loading of 1.2 wt % produced the highest concentration of medium-strong acid sites (6.2 cm3/g STP). X-ray photoelectron spectroscopy and H2 temperature-programmed reduction showed that a Pt loading of 1.2 wt % gave the strongest interaction between Pt nanoparticles and the SAPO-11 support. The Pt@SAPO-11 catalysts were used for the preparation of C8–C17 alkanes by decarboxylation of oleic acid. Employing a reaction temperature of 340 °C, a CO2 atmosphere, a Pt loading on the catalyst of 1.2 wt %, and a reaction time of 4 h, 100% oleic acid conversion was obtained together with an 80% yield of C8–C17 alkanes.

研究领域: 催化化学 · 材料科学
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ACS Applied Energy Materials · 2024 · IF 5.4

In Situ Construction of a Nanostructured Ultrathin Catalyst Layer on Both Sides of a Membrane toward Fuel Cell Application

Huiyuan Liu,Jiaqi Qin,Yang Lv,Zhuo Li,Weiqi Zhang,Qian Xu,Huaneng Su

As the core component, high-performance catalyst-coated membranes (CCMs) are of critical importance for proton exchange membrane (PEM) fuel cells. Composition and microstructure modulations of CCMs are feasible strategies to improve their performance. Herein, an integrated ultrathin ultralow-Pt CCM with a ∼197-nm-thick catalyst layer (CL) and a Pt loading of ∼16 μg cm–2 on each side is directly prepared with a wet-chemical method. The synergistic effect of the precursor and reductant is responsible for the regioselective nucleation and growth of a peony-like Pd nanoflower at the interface of a membrane and reaction solution, followed by the deposition of 4–5 layers of dense Pt nanoparticles on Pd (i.e., Pt/Pd nanoflower CCM). A single cell of the Pt/Pd nanoflower CCM demonstrates a significantly improved mass activity (4.38 A mgPt–1 at 0.9 V) compared with that of the conventional Pt/C CCM (0.22 A mgPt–1). The enhanced performance originates from a high electrochemical active surface area (50.3 and 36.1 m2 gPt–1 for the Pt/C CCM), an increased Pt utilization efficiency (50.4%, 38.7% for the Pt/C CCM), and remarkable oxygen reduction reaction activity (specific activity at 0.9 V: 86.98, 6.09 A m–2 for the Pt/C CCM) closely related to the electronic effect at the Pt and Pd interface. An accelerated degradation test manifests that the prepared Pt/Pd nanoflower CCM is more stable than the conventional CCM. This study opens up a unique avenue to directly engineer nanostructured ultrathin CLs on both sides of a membrane with potential applications in electrochemical energy conversion and storage systems.

CAS / MDL: 50-81-7
研究领域: 材料科学 · 能源工程
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Nature Communications · 2022 ·Vol. 13 ·期 1 ·1-13 · IF 17.694

Low Pt loading for high-performance fuel cell electrodes enabled by hydrogen-bonding microporous polymer binders

Tang Hongying,Geng Kang,Aili David,Ju Qing,Pan Ji,Chao Ge,Yin Xi,Guo Xiang,Li Qingfeng,Li Nanwen

A key challenge for fuel cells based on phosphoric acid doped polybenzimidazole membranes is the high Pt loading, which is required due to the low electrode performance owing to the poor mass transport and severe Pt poisoning via acid absorption on the Pt surface. Herein, these issues are well addressed by design and synthesis of effective catalyst binders based on polymers of intrinsic microporosity (PIMs) with strong hydrogen-bonding functionalities which improve phosphoric acid binding energy, and thus preferably uphold phosphoric acid in the vicinity of Pt catalyst particles to mitigate the adsorption of phosphoric acid on the Pt surface. With combination of the highly mass transport microporosity, strong hydrogen-bonds and high phosphoric acid binding energy, the tetrazole functionalized PIM binder enables an H 2 -O 2 cell to reach a high Pt-mass specific peak power density of 3.8 W mg Pt −1 at 160 °C with a low Pt loading of only 0.15 mg Pt cm −2 .

研究领域: 材料科学 · 能源技术 · 化学工程
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Catalytic dehydrogenation of perhydro-monobenzyltoluene over Pt/Al2O3 for continuous hydrogen release

Changgui Wu,Mengke Xu,Feifei Song,Biao Ma,Fuling Li,Chengxiang Shi,Zhen-Feng Huang,Ruijie Gao,Xiangwen Zhang,Lun Pan,Ji-Jun Zou

Monobenzyltoluene (H0-BT) is a promising liquid organic hydrogen carrier (LOHC), and continuous reaction process represents a more favorable approach in the large-scale hydrogen storage. In this work, the impacts of Pt loading and reaction conditions on the dehydrogenation performance of perhydro-monobenzyltoluene (H12-BT) over Pt/Al 2 O 3 were conducted in a fixed-bed reactor. The results indicate that the dehydrogenation activity of catalyst shows a volcano type as increasing Pt loading, reaching a maximum at 3 wt%. 1 wt% Pt loading is the most appropriate in consideration of the dehydrogenation activity and hydrogen purity. High reaction temperature and low pressure can facilitate dehydrogenation kinetics but result in the undesired byproducts, therefore, the optimal reaction conditions are 320 °C and 0.7 MPa. Additionally, the dehydrogenation performance of H12-BT and perhydro-dibenzyltoluene (H18-DBT) were compared under the similar conditions, revealing that H12-BT may be a superior hydrogen storage carrier.

CAS / MDL: 16941-12-1
研究领域: 化学工程 · 能源科学
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Catalysts · 2023 ·Vol. 13 ·期 10 ·1383 · IF 3.9

The Synthesis of a Pt/SAPO-11 Composite with Trace Pt Loading and Its Catalytic Application in n-Heptane Hydroisomerization

Zhen Jiang,Liduo Chen,Yanhong Cui,Huijie Gao,Yisi Zhou,Wei Zhang,Yanhua Suo,Yingjun Wang

n-Alkane hydroisomerization over bifunctional catalysts is an effective approach for clean fuel production. However, achieving metal–acid synergy and enhancing the catalytic performance by the preparation of bifunctional catalysts with suitable proximity between the metal sites and Brønsted acid sites are still challenging. In this work, a series of Pt/SAPO-11 catalysts with different Pt loading applied inn-heptane hydroisomerization was synthesized. SAPO-11 was synthesized by the Instant Exactness Synthesis (IES) method, which, with unique morphology and pore structure, was chosen as support for the hydroisomerization catalysts; Pt/SAPO-11 was synthesized with the impregnation method, Pt nanoclusters with trace loading were fabricated over the SAPO-11 support, and the as-synthesized catalysts with different Pt loading were labeled as xPt/SAPO-11 (x = 0.1, 0.3, 0.5, 0.8 and 1.0). Various characterizations, including XRD, nitrogen adsorption–desorption, SEM, TEM, NH3-TPD and XPS, were carried out on catalysts to obtain deep insights into the microstructure and valence states of xPt/SAPO-11. The catalytic performance of xPt/SAPO-11, including catalytic selectivity and conversion, was investigated in then-heptane hydroisomerization in detail. Pt loading affected the catalytic properties of xPt/SAPO-11 in the hydroisomerization ofn-heptane. The selectivity of 0.5Pt/SAPO-11 toward isomers was about 65% with a conversion of 77% at 310 °C, which was obviously higher than other xPt/SAPO-11 catalysts.

研究领域: 催化化学 · 能源化学
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Nature Energy · 2021 ·Vol. 6 ·期 6 ·614-623 · IF 60.858

Pt/Fe2O3 with Pt–Fe pair sites as a catalyst for oxygen reduction with ultralow Pt loading

Gao Ruijie,Wang Jian,Huang Zhen-Feng,Zhang Rongrong,Wang Wei,Pan Lun,Zhang Junfeng,Zhu Weikang,Zhang Xiangwen,Shi Chengxiang,Lim Jongwoo,Zou Ji-Jun

Platinum is the archetypal electrocatalyst for oxygen reduction—a key reaction in fuel cells and zinc–air batteries. Although dispersing platinum as single atoms on a support is a promising way to minimize the amount required, catalytic activity and selectivity are often low due to unfavourable O 2 adsorption. Here we load platinum onto α-Fe 2 O 3 to construct a highly active and stable catalyst with dispersed Pt–Fe pair sites. We propose that the Pt–Fe pair sites have partially occupied orbitals driven by strong electronic coupling, and can cooperatively adsorb O 2 and dissociate the O=O bond, whereas OH* can desorb from the platinum site. In alkaline conditions, the catalyst exhibits onset and half-wave potentials of 1.15 V and 1.05 V (versus the reversible hydrogen electrode), respectively, mass activity of 14.9 A mg −1 Pt (at 0.95 V) and negligible activity decay after 50,000 cycles. It also shows better performance than 20% Pt/C in a zinc–air battery and H 2 –O 2 fuel cell in terms of specific energy density and platinum utilization efficiency.

研究领域: 催化 · 电化学 · 材料科学 · 能源存储与转换
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APPLIED ORGANOMETALLIC CHEMISTRY · 2019 ·Vol. 33 ·期 6 ·e4874 · IF 3.259

Platinum(II) complexes bearing bulky Schiff base ligands anchored onto mesoporous SBA-15 supports as efficient catalysts for hydrosilylation

Yingpeng Huo,Jiwen Hu,Shudong Lin,Xingming Ju,Yanlong Wei,Zhenzhu Huang,Yangfei Hu,Yuanyuan Tu

Reported herein is an easy-to-prepare novel heterogeneous catalyst of platinum complexes bearing binary ligands of bidentate naphthalenolimine and cyclo-1,5-octadiene that are anchored onto mesoporous silica SBA-15. The presence of the binary ligands not only stabilized the platinum, but also enabled the platinum atoms to form nanoclusters with diameters of ca 1 nm, and led to high platinum loading (8.69 wt%). Moreover, the platinum catalyst exhibited high catalytic activity towards hydrosilylation of terminal alkenes and styrene with silanes under mild and solvent-free conditions, with excellent regioselectivity.

研究领域: 催化 · 材料科学 · 无机化学
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