APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Hao Zhang,Runze Zhang,Wendi Zhang,Bang Gu,Qinghu Tang,Qiue Cao,Wenhao Fang
Constructing functionalized surface for heterogeneous catalysts is vital toward effective conversion of biomass. We show that Pt nanoparticles (ca. 2.1 nm) loaded on Co-Nb bimetallic oxide can efficiently catalyze the aqueous-phase base-free aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid. We ingeniously construct different surface element-distributions over three Co-Nb oxides (Nb@Co, Co&Nb and Co@Nb) with the same bulk composition by changing precipitation sequence of Co and Nb precursors. This strategy allows rationally modulating synergistic interaction and surface acidity of Co-Nb oxides and in return boosts the pristine oxidation activity of loaded-Pt nanoparticles. We use kinetic investigations, comprehensive characterizations, and particularly in situ DRIFT-IR adsorption technique (CO, pyridine and furfural as probe molecules) to unravel the origin of synergistic catalysis. We disclose that Nb 5+ -enriched surface can formulate sufficient Lewis acidic sites and stabilize electron-rich Pt 0 active centers, accelerating the tandem oxidation of HMF and the intermediates. The Co@Nb-Pt catalyst shows the highest productivity of FDCA (25 mmol FDCA mol Pt –1 h –1 ) among all Pt catalysts in the literature and achieves > 99% yield of FDCA at 110 °C and 10 bar of O 2 .
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Hongxing Yuan,Wei Gao,Jianqi Ye,Tuotuo Ma,Fangyuan Ma,Dan Wen
Modulating the surface properties of electrocatalysts with ligands could effectively regulate their catalytic properties, while limited in-depth understanding of the surface ligands restricted their rational combination. Herein, ionic liquids (ILs) with different lengths of hydrophobic side chains were employed to regulate the surface hydrophobicity of noble metal aerogels, for comprehending the relationship between surface hydrophobicity and oxygen reduction reaction (ORR) activity and enhancing electrocatalytic ORR. The volcano-like trends between the hydrophobicity and the ORR activity for various Pt-based aerogels indicated that a suitable hydrophobic surface constructed by ILs was most favorable for contacting with oxygen molecules and the desorption of oxygen intermediates. Typically, the PtPd aerogel modified by ILs (PtPd aer-[MTBD][PFSI]) exhibited an inspiring ORR activity, with a 70 mV increase in half-wave potential and a 7.1-fold mass activity compared to the commercial Pt/C. Therefore, the regularity between the surface hydrophobicity and ORR activity of noble metal aerogels was uncovered and will facilitate the modulation of electrocatalysts for practical applications.
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PubMed
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
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IF 7.2
Kezhong Wu,FeiFei Nie,Hui Zhao,Xin Qi,Ping Li,Mingxing Wu
The doped transition metal oxides (TMOs) substitute for the traditional Pt as the counter electrode (CE) catalyst is a unique way to reduce the cost and improve the power conversion efficiency (PCE) of dye-sensitized solar cells (DSSCs). Herein, four different morphologies and size of Fe 2 O 3 (nanodiscus (ND), nanocubes (NC), nanorings (NR), nanoball (NB)) assisted by multi-walled carbon nanotube (MWCNT) to prepare Fe 2 O 3 @MWCNT composites, and then were further utilized in the encapsulated DSSCs. The obtained different morphologies Fe 2 O 3 @MWCNT composites had been characterized by X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, and N 2 adsorption-desorption. The significant effects of different morphologies of Fe 2 O 3 on the electrochemical activity of Fe 2 O 3 @MWCNT composites as CEs were confirmed by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and Tafel polarization experiments. The DSSCs using Fe 2 O 3 @MWCNT composites CEs achieved high PCEs of 6.34 (ND), 6.53(NC), 6.65(NR), and 7.09% (NB) to regenerate traditional I 3 − /I − shuttles by the photocurrent-photovoltage ( J - V ) test, respectively, which is due to the synergistic effect between Fe 2 O 3 and MWCNT to improve electrical conductivity and promote a high number of active catalytic sites, implying a remarkable alternative of Pt-free catalyst that can be applied to the encapsulated DSSCs as CEs.
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CATALYSIS COMMUNICATIONS
·
2023
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IF 3.7
Siyue Zhou,Jingjing Fang,Kai Chao,Liang Li
Toluene, dichloromethane, and methanethiol were selected as probe molecules for aromatic, chlorinated, and sulfurated VOCs, respectively, to evaluate the catalytic properties of Pt/CeO 2 composites. The T 90 for toluene, DCM, and methanethiol oxidation were only 153, 265, and 240 °C, when 0.9 wt% Pt/CeO 2 was used as the catalyst. The synergy between Pt and support could be responsible for the high catalytic activity and antipoisoning properties. When combined with NDIR CO 2 sensors, the composite could be used for atmospheric total organic carbon detection. The recorded data almost overlap with that of the theoretical, suggesting the excellent reliability of the dictation system.
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Chemistry-An Asian Journal
·
2022
·Vol. 18
·期 2
·e202201139
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IF 4.839
Fengyun Su,Zhishuai Wang,Mengzhen Tian,Chunxia Yang,Haiquan Xie,Chenghua Ding,Xiaoli Jin,Jiaqi Chen,Liqun Ye
Graphical MoO 2 /g-C 3 N 4 composites were prepared, in which MoO 2 synergetic with Pt photo-deposited during H 2 evolution reaction worked as unilateral dual cocatalyst to improve the photocatalytic activity. The deficient MoO 2 not only promoted visible light absorption of g-C 3 N 4 , but also worked as a “electron pool” to capture and transfer electrons to Pt. Pt is usually used as cocatalyst for g-C 3 N 4 to produce H 2 by photocatalytic splitting of water. However, the photocatalytic performance is still limited by the fast recombination of photo-generated electrons and holes, as well as the poor absorption of visible light. In this work, MoO 2 /g-C 3 N 4 composites were prepared, in which MoO 2 synergetic with Pt photo-deposited during H 2 evolution reaction worked as unilateral dual cocatalyst to improve the photocatalytic activity. Within 4 hours of irradiation, the hydrogen production rate of MoO 2 -Pt dual cocatalyst modified g-C 3 N 4 reached 3804.89 μmol/g/h, which was 120.18 times of that of pure g-C 3 N 4 (GCN, 31.66 μmol/g/h), 10.98 times of that of MoO 2 modified g-C 3 N 4 (346.39 μmol/g/h), and 9.18 times of that of Pt modified g-C 3 N 4 (413.64 μmol/g/h). Characterization results demonstrate that the deficient MoO 2 not only promoted visible light absorption of g-C 3 N 4 , but also worked as a “electron pool” to capture and transfer electrons to Pt.
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Hao Zhang,Xingcong Zhang,Qingdi Sun,Qian He,Hongbing Ji,Xiaohui He
Clarifying the relationship of single metal atom coordination structures and catalytic properties is crucial for the fine-design of highly-efficient catalysts, but systematically manipulating the coordination structure (e.g., coordination numbers (CN) of metal atoms) without changing atomic dispersion is challenging. Herein, we develop a precursor-atomization strategy for the synthesis of single-atom catalysts (SACs) and further precisely tailor Pt-N CN by changing the pyrolysis sequence and atmosphere. It is found that as Pt-N CN decreases (from Pt-N 5 to Pt-N 3 ), the electron density of Pt atoms increases and the energy barrier for H 2 dissociation decreases, thus achieving a ∼550-fold increase in activity of selective hydrogenation of 3-nitrophenylacetylene (reduction of nitro group while maintaining the highly sensitive alkyne group), successfully breaking the selectivity-activity seesaw. Additionally, Pt-N 3 SACs also show remarkably broad applicability for the hydrogenation of nitroarenes (even for iodo-nitrobenzene) due to its unique heterolytic cleavage path of H 2 and preferential adsorption of nitro group.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Jing Lin,Taojin Wang,Jiali Zhou,Xiaodong Wu,Ziran Ma,Shuang Liu
In order to find out the reasons behind the steam-accelerated C 3 H 6 combustion over supported platinum, a Pt@TiO x /TiO 2 catalyst modified by silica (Pt@TiSi) with “super-hydrophilic” surface and metallic platinum sites was synthesized in the present study. In situ spectroscopy analyses excluded the structural change of platinum during reactions, suggesting water has to be involved chemically to accelerate the reactions. By comparing the water response and kinetics of the silica-modified and unmodified samples, a water-mediated O 2 adsorption and activation pathway (HOH···OO* → OOH*) was identified as the origin of the activity bonus induced by steam. Since OOH* formed readily at the interface between platinum and the hydrophilic supports (e.g., TiO x -SiO 2 ), Pt@TiSi exhibited drastically enhanced C 3 H 6 oxidation activity in the presence of moisture. Collectively, this work provides an extensible example about how to fabricate efficient catalysts for reactions with positive H 2 O rate orders, and how to unveil the water effects behind them.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Zengyin Wen,Duojie Wu,Dustin Banham,Ming Chen,Fengman Sun,Zhiliang Zhao,Yiqi Jin,Li Fan,Shaoyi Xu,Meng Gu,Jiantao Fan,Hui Li
Improving the utilization of platinum in proton-exchange membrane (PEM) fuel cells is critical to reducing their cost. In the past decade, numerous Pt-based oxygen reduction reaction catalysts with high specific and mass activities have been developed. However, the high activities are mostly achieved in rotating disk electrode (RDE) measurement and have rarely been accomplished at the membrane electrode assembly (MEA) level. The failure of these direct translations from RDE to MEA has been well documented with several key reasons having been previously identified. One of them is the resistance caused by complex mass transport pathways in the MEA. Herein, we improve the proton and oxygen transportations in the MEA by building a thin and uniform distribution of ionomer on the catalyst surface. As a result, a PEM fuel cell design is capable of showing a current density improvement of 38% at the same voltage (0.6 V) under the H2/air operation.
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FUEL
·
2023
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IF 7.4
Qi Rong,Wenkai Huang,Fuhua Xu,Yanlan Wang,Changlong Wang,Xiang Liu
In spite of significant developments are accomplished in the exploration of H 2 and O 2 evolution upon water electrolysis/photolysis, this remains a challenge to design and develop ideal catalytic systems for this reaction and to isolate H 2 from H 2 -O 2 mixture with membranes. Herein, a series of ZIF-67-supported transition metal nanoparticles (TMNPs/ZIF-67), including Pt, Ir, Pd, Rh, Au and Ag, via immobilization of ultrafine TMNPs at the surface of ZIF-67, have been designed and developed for the selective H 2 generation from NH 3 BH 3 hydrolysis and O 2 evolution upon H 2 O 2 decomposition. In particular, the optimized nanocatalyst Pt/ZIF-67 presents the super-high catalytic property in the both H 2 evolution upon NH 3 BH 3 hydrolysis (689 mol(H 2 )·mol Pt -1 ·min −1 ) and O 2 evolution upon H 2 O 2 decomposition (979 mol(O 2 )·mol Pt -1 ·min −1) at 30 °C. Importantly, the selective “on–off” control for demand-based H 2 generation from NH 3 BH 3 hydrolysis was successfully realized by Zn 2+ /EDTA-2Na system. This highly efficient Pt/ZIF-67 proposed a new method for the promising potential application of ammonia borane and hydrogen peroxide as an economic and safe H 2 resp. O 2 carrier for fuel cell.
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JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Shenghong Wang,Changan Zhou,Yongda Cao,Lei Song,Lirong Zheng,Kui Ma,Hairong Yue
Electrochemical water–gas shift (EWGS) reaction is an emerging technology with energy-saving and environmental-friendly advantages to produce high-purity hydrogen form the waste gas containing CO. However, it remains a significant challenge to design superior activity and highly durable EWGS electrocatalysts, particularly with low content of noble metals. Herein, a series of Pt-xCu/Fe 2 O 3 (x = 0, 2, 5) catalysts are synthesized by the complexation precipitation method to construct coupling sites between Pt and CuOx, aiming to optimize the adsorption of CO and the activation of OH – . The obtained 2.5Pt-2Cu/Fe 2 O 3 catalyst presents a unique Pt-O-Cu structure, delivering a much lowest onset potential, high specific activity, and excellent mass activity (1.5 A·mg Pt -1 ) at 0.73 V ( vs. RHE), which is over 15 and 3 times that of commercial Pt/C (20%) and unmodified Pt/Fe 2 O 3 catalyst, respectively. Meanwhile, the in-situ X-ray absorption results demonstrate that the facilitated interaction among the Pt-O-Cu structure promotes the high durability of the 2.5Pt-2Cu/Fe 2 O 3 catalyst and the operability at high potential. More importantly, the moderate binding of CO and moderate activation of OH* are suggested for boosting the reactivity in the CO electro-oxidation reaction. In particular, the fabricated Pt||2.5Pt-2Cu/Fe 2 O 3 , employed in coupling the HER and CO electro-oxide reaction, shows a remarkable hydrogen production of about 98 mmol H2 ·h −1 ·mg Pt −1 at 0.8 V ( vs. RHE). This work also definitely confirms the possibility of the catalyst being applied to produce hydrogen under practical conditions with different concentrations of CO, even being applied in the purification of trace CO in a hydrogen-rich atmosphere.
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Journal of Physical Chemistry C
·
2022
·
IF 4.177
Dong-Rui Yang,Chen Chi,Miao Ni,Yi-Bai Sun,Xing-Hua Xia
Electrocatalytic water splitting for hydrogen production provides a solution to the problems of energy depletion and environmental pollution. Platinum has been considered as the best catalyst for this reaction; however, its practical application is limited by its high cost and scarcity. Here, we propose a high performance hydrogen evolution reaction (HER) catalyst comprising a single atomic layer of Pt decorated on an Au nanorod surface (AuNRs@SAC-Pt) using a method of underpotential deposition followed by chemical replacement reaction. This catalyst exhibits superior HER activity via maximized electronic interaction with the substrate and gold plasmonic hot carriers. To retain the stability, dispersion, and good conductivity of the catalyst, graphene was used as the support, forming a hybrid (rGO@AuNRs@SAC-Pt). The Pt single atomic layer structure can fully improve the atomic utilization of Pt, maximizing the electronic interaction with the Au substrate, which significantly promotes the HER catalytic performance. The mass activity of rGO@AuNRs@SAC-Pt is 14 times higher than that of the 20% commercial Pt/C catalyst. Meanwhile, the plasmonic hot electrons of AuNRs can further promote the HER performance of Pt single atom as revealed by the significantly decreased overpotential with laser illumination. This research provides new strategies and theoretical guidance for the design of HER catalysts with high atom utilization and excellent catalytic performance.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Lei Li,Zhi-Feng Jiao,Ji-Xiao Zhao,Dan Yao,Xiang Li,Xiang-Yun Guo
The selective hydrogenation of cinnamaldehyde (CAL) is very important, but still remains challenging due to the coexistence of easily hydrogenated C C and C O bonds in CAL molecule. In this work, we report that employing partially oxidized SiC (SiC–O) as the support of Pt can evidently enhance the catalytic selectivity for the selective hydrogenation of C O in CAL. Further investigations show that the partially oxidized SiC surface can change the adsorption mode of CAL and facilitate the selective adsorption of C O in CAL. During the catalytic process, H 2 was dissociated on Pt particles while CAL was mainly adsorbed and activated on the surface of support. The active H species generated on the Pt surface then spilled over to the support surface and reacted with the C O bond activated by the support surface to selectively form cinnamylalcohol. The present work revealed an important cooperative catalysis of metal and SiC, which would be helpful to design and application of more SiC-based catalysts.
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