JOURNAL OF RARE EARTHS
·
2026
·
IF 9.6
Zhengyang Chi,Yonghong Niu,Lin Ma,Yuan Tian,Hao Li
The global transition toward low carbon energy systems has intensified the demand for renewable H 2 and cleaner syngas production. Biomass steam gasification is a promising route, but tar formation and catalyst deactivation still limit its practical application. Herein, Pr 1– x Ce x FeO 3 supported on calcined dolomite was developed for staged biomass steam gasification to couple H 2 production with tar reforming. Statistical screening identifies gasification temperature, Ce substitution level, and steam flow rate as the dominant factors controlling H 2 formation. Under single-factor conditions, Pr 0.6 Ce 0.4 FeO 3 /CD shows the best performance, giving 44.33 vol% H 2 , a total gas yield of 1.51 Nm 3 /kg biomass, a syngas yield of 1.10 Nm 3 /kg biomass, and a syngas fraction of 72.77 vol%. Tar conversion is optimal near 850 °C, where the dry tar yield decreases to 22.75 g/kg biomass, while heavy polycyclic aromatics and >C13 compounds account for 0.79% and 4.14% of the total gas chromatography-mass spectrometry (GC-MS) peak area, respectively. Response surface optimization gives an optimum at 810 °C, x = 0.4, and a steam flow rate of 1.2 mL/min, with an experimental H 2 fraction of 46.22 vol%. Structural and surface analyses indicate that moderate Ce substitution preserves the perovskite framework while regulating defect formation, surface oxygen species, and Fe/Ce/Pr redox behavior. Cycling deactivation is mainly associated with carbonaceous deposits, Fe migration, CaO carbonation, and structural densification. This work provides a feasible perovskite dolomite strategy for integrated tar reforming and production of syngas rich in H 2 from biomass.
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ACS Sustainable Chemistry & Engineering
·
2026
·Vol. 14
·期 29
·13326-13338
·
IF 7.6
Xu Weixin,Wang Songze,Yang Bingcan,Wang Shuomei,Sang Wenqi,Fan Chen,Yan Feng,Tian Sicong,Wen Zongguo,Han Lujia
Converting lignocellulosic biomass to syngas represents a promising way to integrate renewable hydrogen and carbon resources into sustainable carbon-neutral energy systems. However, the conventional biomass gasification process typically relies on excessive steam input, resulting in significant energy penalties and CO 2 emissions. This study proposed a novel integrated gasification process for syngas production from straw, featuring the self-reforming of straw volatiles and utilization of process CO 2 , enabled by the cooperation of Ca(OH) 2 and Fe 2 O 3 . The contents of Ca(OH) 2 and Fe 2 O 3 were optimized to direct straw hydrogen into the volatiles and straw carbon into the solid phase during pyrolysis, thereby facilitating subsequent H 2 and CO production. The cooperation of Ca(OH) 2 and Fe 2 O 3 was manifested in two aspects: generating in situ steam for the self-reforming of volatiles into H 2 and promoting the secondary conversion of biochar and process CO 2 into CO. The optimized C0.3F0.2 reached a syngas yield of 19.3 mmol/g straw with a H 2 selectivity of 35.8% and a CO selectivity of 28.0%. 34.8% of process CO 2 was captured and utilized as CO rather than emitted. This work provides a sustainable and eco-friendly way for converting the hydrogen and carbon resources into efficient syngas production and falls in the domain of carbon-neutral energy system development.
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NANOTECHNOLOGY
·
2020
·Vol. 31
·期 18
·185701
·
IF 3.551
Xiaofeng Cui,Yu Zhou,Jian Wu,Shan Ling,Lijun Zhao,Jianli Zhang,Junwei Wang,Wei Qin,Yuanguang Zhang
A solid-state Z-scheme system, with the synergistic integration of the advantages of various narrow-band semiconductors, is considered to be a potential strategy to develop efficient photocatalysts for operation under visible light illumination. However, the charge separation efficiency of these systems has always been reduced by disordered electron transfer between coupling semiconductors. In this work, we constructed a direct Z-scheme system WO3-MoS2-Pt through the loading of WO3 quantum dots onto MoS2 nanosheets and the selective depositing of a Pt co-catalyst onto MoS2. X-ray diffraction, transmission electron microscopy, atomic electron microscopy and x-ray photoelectron spectroscopy, etc were used to confirm the successful preparation of the targeted photocatalyst. This photocatalytic system showed high visible-light-driven H2 evolution activity (802.2 μmol · h−1 · g−1) and good photostability. Control experiment and mechanism analysis suggested that the remarkable performance can be attributed to the heterojunction formed WO3 and MoS2 and the vectorial electron transfer (WO3 → MoS2 → Pt) achieved by selectively loading the Pt co-catalyst.
研究领域:
材料科学
·
光催化化学
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Small
·
2023
·Vol. 20
·期 20
·2307386
·
IF 13.3
Shiting Wu,Xiaohui Li,Jiaqi Liu,Hanfeng Wu,Hanshuai Xu,Wangfeng Bai,Liang Mao,Xiaowei Shi
Selective photocatalytic production of high-value acetaldehyde concurrently with H 2 from bioethanol is an appealing approach to meet the urgent environment and energy issues. However, the difficult ethanol dehydrogenation and insufficient active sites for proton reduction within the catalysts, and the long spatial distance between these two sites always restrict their catalytic activity. Here, guided by the strong metal-substrate interaction effect, an atomic-level catalyst design strategy to construct Pt-S 3 single atom on ZnIn 2 S 4 nanosheets (Pt SA -ZIS) is demonstrated. As active center with optimized H adsorption energy to facilitate H 2 evolution reaction, the unique Pt single atom also donates electrons to its neighboring S atoms with electron-enriched sites formed to activate the O─H bond in * CH 3 CHOH and promote the desorption of * CH 3 CHO. Thus, the synergy between Pt single atom and ZIS together will reduce the energy barrier for the ethanol oxidization to acetaldehyde, and also narrow the spatial distance for proton mass transfer. These features enable Pt SA -ZIS photocatalyst to produce acetaldehyde with a selectivity of ≈100%, which will spontaneously transform into 1,1-diethoxyethane via acetalization to avoid volatilization. Meanwhile, a remarkable H 2 evolution rate (184.4 µmol h −1 ) is achieved with a high apparent quantum efficiency of 10.50% at 400 nm.
研究领域:
材料科学
·
催化化学
·
能源转化
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Small
·
2026
·
IF 11.8
Wuxi Zhang,Jianyu Li,Yangke Cun,Xinmin Bai,Yingzhu Zi,Zan Xu,Jianbei Qiu,Zhaoyu Ma,Junying Zhang,Zhengwen Yang
Most widely-studied semiconductor catalysts have low efficiency in utilizing near-infrared (NIR) light in the solar spectrum, while also facing major issues such as slow charge-carrier migration rate and lack of active sites that limit photocatalytic performance. Here, a new strategy to promote the solar-light driven photocatalytic activity of ZnIn 2 S 4 was proposed by introducing Rh single atom (SAs) into CeO 2 :Yb,Er/ZnIn 2 S 4 with photo-thermo-electric effects. The introduction of Rh SAs into ZnIn 2 S 4 effectively suppresses charge recombination, and improves reaction rate through photo-thermal effect. CeO 2 :Yb, Er converts NIR light into visible light via up-conversion photo-optical processes and generates high-energy electrons via two-photon photo-electronic process, both of which can activate ZnIn 2 S 4 . Large contact area and strong interface electric field between CeO 2 and ZnIn 2 S 4 enhance photo-electric conversion efficiency. The CeO 2 :Yb,Er/Rh-ZnIn 2 S 4 exhibits a hydrogen production rate of up to 99.68 mmol·g −1 ·h −1 at 10°C and 148.06 mmol·g −1 ·h −1 with non-temperature-controlled conditions. Under mild conditions, the photocatalysts can convert glucose into high-value-added chemicals (e.g., arabinose) while simultaneously generating hydrogen. This work provides a new strategy to improve NIR light utilization efficiency and enhance charge-carrier separation capability through photo-thermo-electric effects, promoting the production of green hydrogen and biomass conversion into high-value-added chemicals.
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高影响因子
JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Hongying Tang,Kang Geng,Jinkai Hao,Xiaojuan Zhang,Zhigang Shao,Nanwen Li
Quaternized poly(sulfone)s based on trimethylamine (PSf-TMA-x) and triethylamine (PSf-TEA-x) are developed to form quaternary ammonium (QA)-biphosphate ion pairs as promising high temperature proton exchange membrane (HT-PEM) in H 2 /O 2 fuel cells. The strong QA-biphosphate ion-pair interaction results in high acid absorption and thus high proton conductivity of 78.1 mS cm −1 for PSf-TEA-110/PA membrane at 160 °C in spite of its lower degree of functionalization. Thus, the peak power density of more than 400 mW cm −2 is achieved at 160 °C for the quaternized PSf membranes in H 2 /O 2 fuel cell, which is higher than that of the poly(benzeimidazole) ( m -PBI) membrane (370 mW cm −2 ). Subsequently, the degradation mechanism of the PSf membranes is demonstrated using NMR technique to be occurred in both the polymer backbone and the QA groups. The stability investigation of model compounds further confirms that the degradation of the membranes resulted from the scission of ether linkage and isopropylidene group and the SN2 nucleophilic substitution of QA at operating conditions. Therefore, the significant performance decrease is observed and the lifetime is only less than 30 h at 200 mA cm −2 which is much lower than that of m -PBI membrane (>40 h).
研究领域:
材料科学
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化学工程
·
能源科学
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yuhao Chen,Kaihang Yue,Jia-Wei Zhao,Zhengyang Cai,Xianying Wang,Ya Yan
Constructing low-cost, high-active and robust heterogeneous hydrogen evolution reaction (HER) electrocatalysts with strong metal–metal oxide-support interaction (SMMOSI) is still an urgent challenge for the development of anion exchange membrane water electrolysis (AEMWE), especially under high current density (e.g., 1 A cm −2 ). Herein, a hierarchical composite of heterogenous Ni 4 Mo/NiMoO 4 (NiMoO x ) nanoparticles (NPs) anchored on a mesoporous carbon CMK-3 (NiMoO x @CMK-3) is designed as a superior electrocatalyst for HER. Significantly, the strong interaction between heterogeneous NiMoO x NPs and CMK-3 supporting matrix effectively stabilize the catalytic active Ni 4 Mo/NiMoO 4 heterostructure by altering the local geometric and electronic structures, leading to maximumly exposure of active sites and promoted electron transfer ability. The optimized electrocatalyst exhibits outstanding HER activity with an extremely low overpotential and Tafel slope of 7 mV@10 mA cm −2 and 27.7 mV dec -1 , respectively, and can steadily operate at 100 mA cm −2 for 800 h. More significantly, owing to these HER merits, the AEMWE configuration with NiMoO x @CMK-3 (−) is also designed, resulting in low cell voltage of 1.965 V@1 A cm −2 and negligible degradation over 400 h@1 A cm −2 . Further ex/in-situ electrochemical spectra evidence that both the partial combined MoO 4 2- from NiMoO 4 and the newly formed MoO 4 2- originating from dissolved Mo in NiMoO x @CMK-3 could boost the fast generation of polymerized Mo 2 O 7 2- that could effectively accelerate the HER process in alkaline conditions by facilitating the formation of active Mo-H* intermediates. Moreover, theoretical calculation results demonstrate the upshifting of d-band center of Mo toward Fermi level for the heterogeneous NiMoO x and the strong charge distribution between the heterointerface could optimize adsorption free energies of H* (ΔG H* ) on the surface of Mo atoms.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xiaoyu Hu,Fengyun Ding,Renjin Xiong,Yongtao An,Xingwen Feng,Jiangfeng Song,Linsen Zhou,Peilong Li,Changlun Chen
Realizing ideal deuterium separation from isotopic mixtures remains a daunting challenge because of their almost identical sizes, shapes, and physicochemical properties. Using the quantum sieving effect in porous materials with suitable pore size and open metal sites (OMSs) enables efficient hydrogen isotope separation. Herein, synthetic HKUST-1-derived microporous mixed-valence Cu(I)Cu(II)-BTC (BTC = benzene-1,3,5-tricarboxylate), featuring a unique network of distinct Cu(I) and Cu(II) coordination sites, can remarkably boost the D2/H2 isotope separation, which has a high selectivity (SD2/H2) of 37.9 at 30 K, in comparison with HKUST-1 and other porous materials. Density functional theory (DFT) calculations indicate that the introduction of Cu(I) macrocycles in the framework decreases the pore size and further leads to relatively enhanced interaction of H2/D2 molecules on Cu(II) sites. The significantly enhanced selectivity of Cu(I)Cu(II)-BTC at 30 K can be mainly attributed to the synergistic effect of kinetic quantum sieving (KQS) and chemical affinity quantum sieving (CAQS). The results reveal that Cu(I) OMSs exhibit counterintuitive behaviors and play a crucial role in tuning quantum sieving without a complex structural design, which provides a deeper insight into quantum sieving mechanisms and a new strategy for the intelligent design of highly efficient isotope systems.
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Catalysts
·
2023
·Vol. 13
·期 7
·1080
·
IF 3.9
Shiyuan Lin,Ruosong He,Wenhang Wang,Yang Wang,Yongqiang Gu,Qiang Liu,Mingbo Wu
The abundant C1 source CO2can be utilized to produce value-added chemicals through hydrogenation technology. A bifunctional catalyst consisting of reducible metal oxide Cr2O3and acidic zeolite ZSM-5 was designed for the direct conversion of CO2+ H2into valuable aromatics, especially para-xylene (PX), via the methanol-mediated pathway. The twin structure of ZSM-5 (ZSM-5T), with sinusoidal channels that are predominantly exposed to the external surface, enhances the possibility of the transformation of methanol into PX due to the favorable diffusion dynamic of PX in the sinusoidal channels. Via the bifunctional catalyst Cr2O3&ZSM-5T, a PX selectivity of 28.7% and PX space-time yield (STY) of 2.5 gCH2h−1kgcat−1are achieved at a CO2conversion rate of 16.5%. Furthermore, we rationally modify the ZSM-5Tzeolite via Cu species doping and amorphous SiO2shell coating (Cu-ZSM-5T@SiO2). After combining with the Cr2O3catalytic component, the CO2conversion (18.4%) and PX selectivity (33.8%) are increased to some extent, which systematically increases the STY of PX to 3.0 gCH2h−1kgcat−1. The physicochemical property of the acidic zeolite and the corresponding structure-function relationship in enhancing the PX productivity are discovered. Our work provides a novel catalyst design idea to boost PX synthesis performance from CO2hydrogenation.Keywords:CO2hydrogenation;bifunctional catalysts;para-xylene;H-ZSM-5 zeolites
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CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Yingcong Wei,Qiqi Zhang,Ying Zhou,Xiongfeng Ma,Lele Wang,Yanjie Wang,Rongjian Sa,Jinlin Long,Xianzhi Fu,Rusheng Yuan
Simultaneous generation of H 2 fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical energy. Herein, for realizing UV-visible-NIR light driven dehydrogenation of benzyl alcohol (BA) into benzaldehydes (BAD) and H 2 , a novel localized surface plasmon resonance (LSPR) enhanced S-scheme heterojunction was designed by combining noble-metal-free plasmon MoO 3– x as oxidation semiconductor and Zn 0.1 Cd 0.9 S as reduction semiconductor. The photoredox system of Zn 0.1 Cd 0.9 S/MoO 3– x displayed an unconventional reaction model, in which the BA served as both electron donor and acceptor. The S-scheme charge transfer mechanism induced by the formed internal electric field enhanced the redox ability of charge carriers thermodynamically and boosted charge separation kinetically. Moreover, due to the LSPR effect of MoO 3− x nanosheets , Zn 0.1 Cd 0.9 S/MoO 3− x photocatalysts exhibited strong absorption in the region of full solar spectrum. Therefore, the Zn 0.1 Cd 0.9 S/MoO 3− x composite generated H 2 and BAD simultaneously via selective oxidation of BA with high production (34.38 and 33.83 mmol·g −1 for H 2 and BAD, respectively) upon full solar illumination. Even under NIR light irradiation, the H 2 production rate could up to 94.5 mmol·g −1 ·h −1 . In addition, the Zn 0.1 Cd 0.9 S/MoO 3– x composite displayed effective photocatalytic H 2 evolution rate up to 149.2 mmol·g −1 ·h −1 from water, which was approximate 6 times that of pure Zn 0.1 Cd 0.9 S. This work provides a reference for rational design of plasmonic S-scheme heterojunction photocatalysts for coproduction of high-value chemicals and solar fuel production.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Hongcai Su,Tian Li,Shurong Wang,Lingjun Zhu,Yanjun Hu
The accumulation and improper disposal of a large amount of plastic waste have exacerbated the deterioration of the global ecosystem and environment. To simplify the complex management system and alleviate the environmental impact of plastic wastes, this study reports a novel one-pot hydrothermal conversion strategy for polyethylene terephthalate (PET), integrating three steps, namely depolymerization , subsequent in-situ aqueous phase reforming, and in-situ CO 2 capture. Here, the PET waste was converted directly into the clean high-purity H 2 fuel and the disodium terephthalate (Na 2 -TPA). A high yield of H 2 at 23.7 mol/kg PET with ca. 99 % of H 2 concentration was obtained at a temperature as low as 240 °C. The feasibility of this strategy in handling real-world PET plastic wastes was demonstrated through a series of tests on beverage bottles, food packaging, and polyester fabric waste. The Na 2 -TPA crystals produced from the proposed PET conversion system exhibited purity close to that of the standard sample, and thus had the potential to be directly used as an electrode material . Overall, this strategy provides an efficient way to transform PET waste into high-value products and improves the sustainability of the PET waste disposal process.
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高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 153
·期 8
·2517-2526
·
IF 2.936
Wu Jindong,Zuo Jianliang,Liu Kuiliang,Lin Jing,Liu Zili
Designing a stable, efficient, highly selective, and low-cost dehydrogenation catalyst, using formic acid to produce hydrogen energy, is challenging even today. This paper reports a facile preparation method of constructing Pd–Co alloy-composite catalyst for hydrogen production using formic acid by heterogeneous catalyst decomposition. The results demonstrate that introducing a nonprecious cobalt metal could significantly reduce precious palladium metal usage. Moreover, the particle size reduces from 13.50 nm (without Co) to 3.4 nm (with Co). More importantly, the Pd 2+ amount in the catalyst affect the catalytic decomposition of formic acid to produce hydrogen. Additionally, Pd 0.9 Co 0.1 /C 650 exhibits excellent catalytic activity and cyclic catalytic stability and it is one of the best non-precious metal doped Pd-based catalysts. The development of a synthetic method with the addition of nonprecious metal in this paper opens up a new avenue for cheap and efficient catalysts for application scenarios of hydrogen production. H 2 production by formic acid dehydrogenation. Graphical abstract
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危险品化学品经营许可证（带存储）