INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Chengqi Feng,Yuewen Dai,Chenkai Jin,Juncheng Huang,Jinhang Yang,Yifei Huang,Haining Na,Jin Zhu
Efficient conversion of cellulose to glucose is a crucial challenge for the energy and materialization of non-food biomass. Solid acids' adsorption strength is essential to affecting mass transfer efficiency. In this study, solid acids with different particle sizes (from 0.25 to 10.10 μm) modified with -OH and -PO 3 H 2 were obtained by hydrothermal method. Hydrolysis of cellulose at 180 °C for 4 h revealed that the particle size of the solid acids was directly proportional to the cellulose conversion (R 2 = 0.925). Still, there was no significant correlation with the glucose yield (R 2 = 0.632). Eventually, the cellulose conversion reached 98.9 %, with a 30 % glucose yield. The solid acids demonstrated good stability and recoverability. This study fills the gap in the influence of solid acid particle size and reveals the mechanism of strong adsorptive mass transfer and hydrolysis efficiency. It provides the theoretical basis for the design of high-performance solid acids.
研究领域:
生物化学
·
能源材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Ying Huo,Xuyu Wang,Zebao Rui,Xiaoqing Yang,Hongbing Ji
Insight into the relationship between catalytic trends and physicochemical properties of composite nanoparticles is essential for their rational design. Herein, a series of 3d-M (M = Mn, Fe, Co, Ni) metal hydroxide-promoted PtM(OH)x/Al2O3 catalysts are developed and well characterized for establishing the catalytic HCHO oxidation reactivity trend as a function of more fundamental properties, such as hydroxyl concentration and adsorption strength. The reactivity of PtM(OH)x/Al2O3 exhibits an increasing trend of Mn < Fe < Co < Ni, which is governed by their OH–M2+δ bond strength (Ni < Co < Fe < Mn) and surface hydroxyl concentration (Mn < Fe < Co < Ni). Both PtCo(OH)x/Al2O3 and PtNi(OH)x/Al2O3 exhibit a (>)95% HCHO conversion and (>)100 h performance stability at 30 °C with a low 0.2 wt % Pt loading amount. The identification of these catalytic trends provides foundations for composite active sites design for HCHO oxidation and other hydroxyl-involved reactions.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Minmin Wang,Chao Feng,Xin Zhang,Ping He,Houyu Zhu,Yunqi Liu,Yuan Pan
The development of atomically dispersed platinum-based catalysts with high performance and well-defined active site structures is crucial for the commercialization of water electrolysis for hydrogen production. Herein, we propose a coordination dual-shell synergistic regulation mechanism of coal pitch-derived carbon-supported single atom Pt-N x O y -S 1 catalytic sites by a self-assembly-pyrolysis strategy for promoting hydrogen evolution reaction (HER). The Pt-N 3 O 1 -S 1 sites exhibited the highest HER performance, with an overpotential of 92 mV at a current density of 400 mA cm −2 . At 50 mV, the turnover frequency was 34.04 s −1 and the mass activity was 22.83 A mg Pt −1 , which is 63.4 times that of the 20% Pt/C catalyst. Theoretical calculations revealed that the coordination dual-shell impacts the electronic structure of the Pt atoms and the adsorption strength towards reactants synergistically. The S atoms in the second coordination shell weakened the strength of Pt-N first shell, resulting the more surface valence electrons around Pt atoms, exhibiting the most suitable adsorption free energy and enhancing the adsorption of H + on Pt-N 3 O 1 -S 1 sites, thus enhancing the electrocatalytic HER process by promoting Volmer step. This work reveals that coordination dual-shell synergistic regulation is an effective strategy for enhancing the electrocatalytic reaction process.
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
·
2022
·
IF 12.92
Guang Gao,Zelun Zhao,Jia Wang,Yongjie Xi,Peng Sun,Fuwei Li
ABSTRACT Engineering the surface microenvironment by tuning the binary interactions between a supported metal with a secondary metal oxide (MO x ) or support has been a common method for improving the catalytic performance of supported metal catalysts. However, few studies have investigated the ternary interactions among the metal, MO x , and support. Here, we report for the first time the formation of metal-MO x -support interaction (MMSI) in reducible TiO 2 -supported PtReO x catalysts, affording 87% yield and 100% ee in the tandem hydrogenation of an aqueous chiral cyclohexane-1,2-dicarboxylic acid into the corresponding diol; the catalytic activity is eight times higher than that obtained with non-reducible support counterparts in the same reaction via traditional batch synthesis with multiple steps and unfriendly reagents. Detailed experimental and computational studies suggest that the TiO 2 crystalline phase-dependent density of the oxygen vacancies induces different Pt-ReO x -TiO 2 interactions, which dominate the electron transfer therein and tune the adsorption strength of the carbonyl moiety of the substrate/intermediate, thus promoting the hydrogenation activity and selectivity. In addition, the strong MMSI endows the optimal rutile TiO 2 supported PtReO x catalyst with an outstanding lifetime of 400 h in a fixed-bed reactor under acidic aqueous conditions and ensures efficient applications in the selective hydrogenation of aliphatic dicarboxylic acids and functional carboxylic acids. This work provides a promising strategy for the development of efficient and stable supported catalysts for the selective hydrogenation of diverse C–O and C=O bonds.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2024
·
IF 18.9
Zhe Bai,Zhenhua Wang,Tan Wang,Zeyu Wu,Ruilong Li,Xiaotian Gao,Yu Bai,Kening Sun
The partially filled d orbital of transition metal-based catalysts demonstrate excellent catalytic activity against polysulfides. However, an appropriate descriptor to reveal their structure-activity relationship is lacked. This study proposes a quantitative relationship between the e g occupancy of perovskite oxides and polysulfide catalytic activity, serving as an activity descriptor. LaCoO 3 , with a moderate e g occupation (t 2g 5 e g 1.08 ), demonstrates effective polysulfide anchoring and facilitated redox kinetics conversion compared to LaCrO 3 (t 2g 3 e g 0 ) and LaFeO 3 (t 2g 3 e g 2 ), showcasing exceptional catalytic performance. The degree of e g occupancy significantly influences the polysulfides adsorption strength, with empty or fully filled e g orbitals resulting in either strong or weak adsorption, respectively. LaCoO 3 -based batteries exhibit remarkable reversible capacity over 700 cycles at 1.0C, with a minimal capacity fading rate of 0.065 % per cycle. This work elucidates the crucial role of e g descriptor for evaluating the adsorption and conversion on polysulfides, offering insights into the development of innovative lithium-sulfur electrocatalysts.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Aiqun Kong,Menghui Liu,Houjun Zhang,Zifan Cao,Jinli Zhang,Wei Li,You Han,Yan Fu
Cyclohexanecarboxylic acid (CCA), an important chemical and pharmaceutical intermediate, is commonly produced from thermal catalytic hydrogenation of benzoic acid (BA) under high temperature and pressure. Herein, electrocatalytic hydrogenation (ECH) for highly selective conversion of BA into CCA using carbon fibers with different graphitization degree (carbon fiber paper (CFP), carbon fiber cloth (CFC)) supported commercial platinum carbon (Pt/C) electrode was reported for the first time without using external H 2 . Our experimental results show that, at room temperature and 1 atm, the BA conversion and the CCA selectivity are both as high as 100% in 0.05 M H 2 SO 4 over carbon fiber paper (CFP)-supported Pt/C (Pt/C/CFP). Meanwhile, Pt/C/CFP electrode still maintains outstanding stability after 10 reaction cycles. In situ Raman results and theoretical calculations reveal that the adsorption strength of BA over Pt/C/carbon fibers electrode varies with the graphitization degree of carbon fibers along with the applied potential. The superior ECH performance of the Pt/C/CFP is mainly attributed to the high dispersity of Pt/C catalysts on CFP as well as unique electronic interaction, which improved the adsorption and activation of BA. Typically, CFP with few defects can induce the accumulation of electrons around the Pt regions and enhance the electron-deficient aromatic adsorption thus improving the ECH performance of Pt/C/CFP, which is the opposite for CFC with more defects.
研究领域:
电化学
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催化
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材料科学
·
化工
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yiyi Ju,Aichuang Zhang,Zhenyu Xu,Yuan Liu,Xiaorong Zhu,Peng Zhu,Luozeng Zhou,Xiaolei Yuan
High-entropy alloy aerogels (HEAAs) have become promising electrochemical catalysts because of the advantageous combination of high-entropy alloys and aerogel structure. However, how to fabricate 3D porous high-entropy alloys accurately is still a great challenge due to their inherent thermodynamic instability and differences in reduction potentials of metal ions. Herein, PtBi 1.5 Ni 0.2 Co 0.2 Cu 0.2 HEAAs have been synthesized by combining co-reduction method and freeze-drying technology. The resulting PtBi 1.5 Ni 0.2 Co 0.2 Cu 0.2 HEAAs have the structural and morphological benefits of both high-entropy alloys and aerogels. Both XPS and DFT results confirm that the d-band center of PtBi 1.5 Ni 0.2 Co 0.2 Cu 0.2 HEAAs shifts to lower binding energy compared to Pt/C, indicating the effective regulation of electronic structure on the surface of PtBi 1.5 Ni 0.2 Co 0.2 Cu 0.2 HEAAs. As a demonstration in the methanol oxidation reaction (MOR), a mass activity of 4.19 A mg Pt −1 and long-term stability (>0.33 A mg Pt −1 after 10 cycles of 3600 s stability test) can be obtained on the PtBi 1.5 Ni 0.2 Co 0.2 Cu 0.2 HEAAs, outperforming binary Pt-based alloys and commercial Pt/C. The CO adsorption strength of PtBi 1.5 Ni 0.2 Co 0.2 Cu 0.2 HEAAs is more weaker than that of PtBi 1.5 alloys and Pt/C, which proves the enhanced CO tolerance. The results pave the way for fabricating the hybrids of high-entropy alloys and aerogels with superior activity and stability.
研究领域:
材料科学
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电化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Long Daojun,Liu Yongduo,Ping Xinyu,Chen Fadong,Tao Xiongxin,Xie Zhenyang,Wang Minjian,Wang Meng,Li Li,Guo Lin,Chen Siguo,Wei Zidong
The serious problem of carbon monoxide (CO) poisoning on the surface of Pt-based catalysts has long constrained the commercialization of proton exchange membrane fuel cells (PEMFCs). Regeneration of Pt sites by maintaining CO scavenging ability through precise construction of the surface and interface structure of the catalyst is the key to obtaining high-performance CO-resistant catalysts. Here, we used molybdenum carbide (MoC x ) as the support for Pt and introduced Ru single atoms (SA-Ru) at the Pt-MoC x interface to jointly decrease the CO adsorption strength on Pt. More importantly, the MoC x and SA-Ru are immune to CO poisoning, which continuously assists in the oxidation of adsorbed CO by generating oxygen species from water dissociation. These two effects combine to confer this anode catalyst (SA-Ru@Pt/MoC x ) remarkable CO tolerance and the ability to operate stably in fuel cell with high CO concentration (power output 85.5 mW cm −2 @20,000 ppm CO + H 2 – O 2 ), making it possible to directly use the cheap reformed hydrogen as the fuel for PEMFCs.
研究领域:
材料科学
·
电化学
·
催化
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Chong Yao,Jiwei Wu,Limei Pan,Lu Yu,Jie Luo,Jinjin Shan,Jie Liu,Chunshan Lu,Feng Feng,Xiaoliang Xu,Lili Lin,Yuxue Yue,Qingtao Wang,Jia Zhao,Qunfeng Zhang,Xiaonian Li
N-doped carbon materials were synthesized using a straightforward salt template method for Pt metal modification, resulting in a reduction in particle size from 4.8 nm to 2.1 nm due to the interaction between Pt and the carrier. The hydrogenation activity of nitrobenzene increased by 4.5 times compared to undoped catalysts. Additionally, the electronic effects of N and Pt enhanced the selectivity of p-aminophenol by up to 20.4 %. The anchoring of Pt by N improved the stability of active metal centers in a strong acidic system, thereby retarding Pt loss. Theoretical calculations and characterization revealed that the enhancement of activity relied on the high dispersion of Pt, while the improvement in product selectivity was associated with changes in the adsorption strength of the phenylhydroxylamine intermediate. N anchoring of Pt, inducing an electron effect, disentangled the activity and selectivity of nitrobenzene hydrogenation for the preparation of p-aminophenol.
研究领域:
催化
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
ELECTROCHEMISTRY COMMUNICATIONS
·
2020
·
IF 4.333
Xin Zong,Jie Zhang,Jinqiu Zhang,Wen Luo,Andreas Züttel,Yueping Xiong
The electrochemical reduction of carbon dioxide (CO 2 RR) has attracted enormous interest because of the energy crisis and climate change; however, more efficient catalysts are required for practical applications. Herein, we present electrospinning as a facile strategy to synthesize a three-dimensional network of carbon nanofibers embedded with Cu and CeO x nanoparticles (Cu/CeO x @CNFs) as a CO 2 RR catalyst. The Cu–CeO x interface produced using this method offers synergistic geometric and electronic effects which optimize the adsorption strength of reaction intermediates for the electroreduction of CO 2 to CO. In a flow cell configuration, a current density of 100 mA cm −2 and a CO faradaic efficiency of 59.2% can be obtained at −0.60 V vs. RHE.
研究领域:
电化学
·
材料科学
·
催化
·
纳米技术
·
能源转换
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 25
·2301343
·
IF 19
Ping Yan,Tao Yang,Minxi Lin,Yanan Guo,Zipeng Qi,Qiquan Luo,Xin-Yao Yu
Layered metal hydroxides (LMHs) are promising catalysts for oxygen evolution reaction. However, the hydrogen evolution reaction (HER) activity of LMHs is unsatisfactory due to their poor conductivity and limited active sites. Herein, taking Ni(OH) 2 as demonstration, a novel “one stone five birds” plasma activation strategy synergistic with Ru single atoms (Ru SAs) doping is developed to boost the HER activity of Ni(OH) 2 by constructing heterostructured β-Ni(OH) 2 /Ni-Ru SAs nanosheet arrays (NSAs). Benefiting from the structural/compositional features and optimized electronic state, the as-obtained β-Ni(OH) 2 /Ni-Ru SAs NSAs exhibit splendid HER activity with a low overpotential of 16 mV at 10 mA cm −2 and a small Tafel slope of 21 mV dec −1 in alkaline solution. Excellent HER performance in alkaline seawater and neutral solutions are also demonstrated by the β-Ni(OH) 2 /Ni-Ru SAs NSAs. The plasma activation and Ru SAs doping play important roles in enhancing water adsorption and accelerating the kinetics of water dissociation. Density functional theory (DFT) calculations reveal that the introduction of Ru SAs in the system facilitates the generation of surface OH vacancies for providing more active sites as well as decreases the antibonding state density of the generated mid-gap state for enhancing H adsorption strength toward the optimal range.
研究领域:
材料科学
·
电化学
·
催化
·
能源材料
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）