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SOLAR ENERGY · 2018 · IF 4.374

Preparation of meso-Ag/Al2O3 and synergistic water disinfection of metallic silver and ROS under visible light

Huajun Chen,Wenjie Tian,Wuxiu Ding

Metallic sliver-doped mesoporous Al 2 O 3 fibers (meso-Ag/Al 2 O 3 ) that can harvest visible light to speed up solar water purification, were synthesized by one-pot hydrothermal method. Insightful analyses of XRD, XRF and XPS of meso-Ag/ Al 2 O 3 verified that metallic silver occupied interstitial positions of Al 2 O 3 lattice forming interstitial solid solution. N 2 adsorption/desorption illustrated that meso-Ag/Al 2 O 3 exhibited significantly increases in the specific surface area, pore volume and average pore diameter after doping with silver. The UV–Vis diffuse reflectance spectra and disinfection performance indicated that meso-Ag/Al 2 O 3 can harvest visible light to promote the conversion of dioxygen to ROS for water disinfection compared with the widely used TiO 2 . With our approach, we achieved water disinfection of >99.999% inactivation of bacteria in 120 min with a small amount of material (8 mg/L) under simulated visible light.

CAS / MDL: 7761-88-8
研究领域: 环境科学 · 材料科学 · 水处理
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ACS Sustainable Chemistry & Engineering · 2020 · IF 7.632

Vacancy-Enabled Mesoporous TiO2 Modulated by Nickel Doping with Enhanced Photocatalytic Nitrogen Fixation Performance

Jiaxin Li,Dandan Wang,Renquan Guan,Yujun Zhang,Zhao Zhao,Hongju Zhai,Zaicheng Sun

Photocatalysis provides a sustainable route to convert N2 to NH3 with the aid of a photogenerated electron. Beyond the typical issue in the photocatalytic field, NH3 synthesis requires adsorption, activation, and hydrogenation of N2. In this report, Ni-doped TiO2 (Ni-x-TiO2) photocatalysts were fabricated by a simple sol–gel method to introduce the oxygen defects and Ni site on TiO2. The oxygen vacancy (Vo) enhances the adsorption of N2 on the catalyst surface. The Ni doping induced a defect energy level below the conduction band, which prefers to accept the photogenerated electron. The electron captured by Vo tends to transfer to the adsorbed N2 and activate N2. On the other hand, the Ni site is a typical H2 production site. It provides enough H2 for the hydrogenation of N2 to form NH3. To sum up all of these advantages, Ni-doped TiO2 displays a high NH3 production rate of 46.80 μmol·g–1·h–1 which is about 7 times higher than that of pure TiO2. This manuscript provides a potential method to design a highly efficient photocatalyst for the NH3 synthesis.

研究领域: 材料科学 · 催化 · 化学工程 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

In-situ decoration of unsaturated Cu sites on Cu2O photocathode for boosting nitrogen reduction reaction

Ying Liu,Hongye Bai,Qianxiao Zhang,Yajie Bai,Xuliang Pang,Fagen Wang,Yingchen Yang,Jinrui Ding,Weiqiang Fan,Weidong Shi

Photoelectrochemical N 2 reduction reaction (PEC NRR) into chemical energy source is a promising technique for solving environmental challenges and the energy crisis, which depends on the exploration of p-type photocathodes. Cu 2 O is a p-type semiconductor, which can be applied as a photocathode for PEC NRR. However, the adsorption and activation ability of N 2 over the pristine Cu 2 O is still not ideal, causing the overall efficiency far below the theoretical value. In this work, we first proposed a feasible strategy to in-situ modify the surface of Cu 2 O with Cu-MOF, and the Cu-MOF/Cu 2 O heterostructure exhibited the significantly boosted NH 3 production rate (7.16 mmol/m 2 /h). The ultra-thin Cu-MOF film takes a nature of porous structure and unsaturated Cu sites, contributing to a favorable interface environment for the adsorption and activation of N 2 . The N 2 temperature programmed desorption and contrast photocurrent curves revealed the desirable selectivity for PEC NRR, and the isotope NMR further confirmed the accuracy of NH 3 evolution process. Therefore, the organic–inorganic hybrid systems built from Cu-MOF and Cu 2 O would offer a new insight for establishing the efficient PEC NRR system.

CAS / MDL: 554-95-0
研究领域: 材料科学 · 环境科学 · 化学工程
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Nanoscale · 2023 ·Vol. 15 ·期 8 ·4071-4079 · IF 6.7

Introducing oxygen vacancies in a bi-metal oxide nanosphere for promoting electrocatalytic nitrogen reduction

Heen Li,Xiaoyue Xu,Xiaohu Lin,Jianmin Chen,Kunling Zhu,Fei Peng,Faming Gao

The sluggish breakage of the N–N triple bond, as well as the existence of a competing hydrogen evolution reaction (HER), restricts the nitrogen reduction reaction process. Modification of the catalyst surface to boost N2 adsorption and activation is essential for nitrogen fixation. Herein, we introduced surface oxygen vacancies in bimetal oxide NiMnO3 by pyrolysis at 450 °C (450-NiMnO3) to achieve remarkable NRR activity. The NiMnO3 3D nanosphere with a rough surface could increase catalytically active metal sites and introduce oxygen vacancies that are able to enhance N2 adsorption and further improve the reaction rate. Benefiting from the introduced oxygen vacancies in NiMnO3, 450-NiMnO3 showed excellent performance for nitrogen reduction to ammonia with a high NH3 yield of 31.44 μg h−1 mgcat−1 (at −0.3 V vs. RHE) and a splendid FE of 14.5% (at −0.1 V vs. RHE) in 0.1 M KOH. 450-NiMnO3 also shows high long-term electrochemical stability with excellent selectivity for NH3 formation. 15N isotope labeling experiments further verify that the source of produced ammonia is derived from 450-NiMnO3. The present study opens new avenues for the rational construction of efficient electrocatalysts for the synthesis of ammonia from nitrogen.

研究领域: 电化学 · 催化 · 材料科学 · 化学工程
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FUEL · 2022 · IF 8.035

SAPO-11 molecular sieves synthesized in alcohol-water concentrated gel system with improved acidity, mesoporous volume and hydroisomerization performance

Xiaojun Dai,Yan Cheng,Meng Si,Qiang Wei,Dongdong Chen,Wenbin Huang,Yasong Zhou

A series of SAPO-11 molecular sieves were synthesized in the concentrated gel system by reducing the water content in the synthesis system. With SAPO-11 molecular sieves as supports, NiW-supported catalysts were prepared for the hydroisomerization of n-hexadecane. SAPO-11 molecular sieves and catalysts were characterized by XRD, SEM, N 2 adsorption–desorption, NH 3 -TPD, Py-IR, HRTEM and XPS. The results showed that reducing the water content in the synthesis system could increase the mesoporous volume of SAPO-11 molecular sieve and improve the acidity of SAPO-11. For the corresponding catalysts, using SAPO-11 synthesized in concentrated gel system as the support weakened the interaction between the active phase and the support, and increased the dispersion and stacking number of the active phase, which effectively improved the catalytic performance of the catalyst. The yield of i-hexadecane of the catalyst NiW/45W-SA corresponding to SAPO-11 synthesized in conventional water content system was 28.14%, while that of the catalyst NiW/5W-SA corresponding to SAPO-11 synthesized in concentrated gel system was 52.24%. According to the distribution of isomers, it is inferred that hydroisomerization of n-hexadecane over NiW/SAPO-11 follows the pore-mouth mechanism.

研究领域: 催化 · 材料科学 · 化学工程
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MATERIALS CHEMISTRY AND PHYSICS · 2019 · IF 2.781

Hierarchical Ti-containing hollownest-structured zeolite synthesized by seed-assisted method for catalytic epoxidation of alkenes efficiently

Yun Yang,Tianjun Zhang,Dan Zhou,Xinchao Liu,Shuijin Yang,Xinhuan Lu,Qinghua Xia

Recently, a Ti-containing hollownest-structured zeolite (Ti-HSZ) material with the shell constructed by randomly intergrown MWW (framework type code) flaky crystals has been synthesized through one-step rotating hydrothermal method within 3.5 days, which shows predominant catalytic property for the epoxidation of alkenes . Herein, it is firstly reported that the crystallization efficiency of Ti-HSZ material can be notably increased by applying seeds-assisted synthesis method. Thus-crystallized materials have been characterized by XRD , UV–vis, XPS , SEM , TEM, FT-IR, and N 2 adsorption-desorption. Moreover, the key controlling factors are revealed to include the addition percentage of seed crystals, rotating rate and filling degree of autoclave. When 2 wt% or 3 wt% seed crystals are added into the reaction gel, the crystallization time of Ti-HSZ can be sharply reduced to 2.5 days or even 2.0 days, respectively. Particularly, thus-synthesized Ti-HSZ-SM material still maintains hollownest morphology characteristic and excellent catalytic activity and catalytic stability. About 95% allyl chloride can be converted into corresponding epoxide when using H 2 O 2 as oxidant, and about 85% cyclopentene and 87% cyclooctene can be converted into corresponding epoxides when using TBHP as oxidant, with the selectivity for epoxides of nearly 100%.

研究领域: 催化 · 材料科学 · 化学工程
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Catalysts · 2023 ·Vol. 14 ·期 1 ·18 · IF 3.9

Cerium Doping Effect in 3DOM Perovskite-Type La2−xCexCoNiO6 Catalysts for Boosting Soot Oxidation

Kaixuan Chen,Linsheng Xu,Yuanfeng Li,Jing Xiong,Dawei Han,Yaxiao Ma,Peng Zhang,Haoqi Guo,Yuechang Wei

Herein, we present an in-depth investigation into the enhancement of catalytic soot oxidation through cerium-doped three-dimensional ordered macroporous (3DOM) La-Co-Ni-based perovskites synthesized with the colloidal crystal template (CCT) method. The 3DOM structure significantly contributes to the accessibility and interaction efficiency between soot and catalyst. Based on the results of powder X-ray diffraction (XRD), N2adsorption-desorption measurements, scanning electron microscopy (SEM), temperature-programmed oxidation of NO (NO-TPO), temperature-programmed reduction of H2(H2-TPR), in situ infrared Fourier transform spectroscopy (In-situ DRIFTS), and temperature-programmed oxidation (TPO) reactions, the role of cerium doping in modifying the structural and catalytic properties of 3DOM perovskite-type La2−xCexCoNiO6catalysts was investigated systematically. The optimized cerium doping ratio in La2−xCexCoNiO6catalysts can improve the microenvironment for efficient soot-catalyst contact, enhancing the catalytic activity of soot oxidation. Among the catalysts, the 3DOM La0.8Ce1.2CoNiO6catalyst shows the highest catalytic activity for soot oxidation, whose T10, T50, and T90values are 306 °C, 356 °C, and 402 °C, respectively. The mechanism of the cerium doping effect for boosting soot oxidation is proposed: The doping of Ce ions can increase the surface oxygen species, which is the main active species for promoting the key step of NO oxidation to NO2in catalyzing soot oxidation. This research provides a new strategy to develop high-efficient non-noble metal catalysts for soot oxidation in pollution control and sustainable environmental practices.

研究领域: 催化 · 环境科学 · 材料科学
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ENERGY & FUELS · 2023 · IF 5.3

Deep Hydroisomerization of n-Hexadecane over NiWS/SAPO-11 Catalyst: Size Effect of the Support and Revelation of the Reaction Network

Xiaojun Dai,Yan Cheng,Tingting Liu,Lingjuan Mao,Qiang Wei,Yasong Zhou

SAPO-11 molecular sieves with different crystal sizes and particle sizes, especially nanosized small-crystal SAPO-11 molecular sieves, were successfully synthesized, and the corresponding NiWS-supported catalysts were prepared for the hydroisomerization of n-hexadecane. XRD, SEM, N2 adsorption–desorption, Py-IR, and HRTEM were used to analyze the effects of crystal size and particle size of the supports on their physicochemical properties, active phase properties, and catalytic performance of the catalysts. Through reaction evaluation and analysis of isomeric products, the effects of the size change of the support on the hydroisomerization performance of the catalyst and the hydroisomerization depth of n-hexadecane were determined. Through comprehensive analysis of the cracking products, it was determined that secondary cracking occurred when the conversion of n-hexadecane on the NiW/SAPO-11-S catalyst reached about 42.7%, and the secondary isomerization occurred when the conversion of n-hexadecane reached about 80%. The hydroisomerization reaction network of n-hexadecane over the NiWS/SAPO-11 catalyst was studied emphatically, and it was found for the first time that the secondary cracking of n-hexadecane during hydroisomerization followed the C3-β-scission mechanism.

研究领域: 化学工程 · 催化 · 材料科学
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Biomass Conversion and Biorefinery · 2022 · IF 4.05

Electroplating sludge-derived magnetic copper-containing catalysts for selective hydrogenation of bio-based furfural

Xiao Yaoxin,Zhang Jun,Zhu Lingjun,Shan Rui,Yuan Haoran,Chen Yong

A series of inexpensive electroplating sludge-derived magnetic copper-containing catalysts were developed for the selective hydrogenation of biomass-based furfural (FFR) into furfuryl alcohol (FA) and 2-methylfuran (MF). The specific structural characteristics of as-prepared magnetic copper-containing samples were clearly identified through various techniques, including XRD, XPS, N 2 adsorption–desorption, NH 3 -TPD, SEM and so on. The characterizations revealed that the hydrogen pre-activated magnetic catalysts supplied metallic Cu species, medium acidity and porosity for the catalytic upgrading of FFR in hydrogen atmosphere. As for FFR-to-FA as well as FFR-to-MF transformations, the magnetic copper-containing catalyst with calcination temperature of 800 °C exhibited excellent performance towards the formation of FA and MF, wherein desirable FA yield of 98.5 mol% and MF yield of 71.3 mol% were achieved at reaction temperatures of 160 °C and 240 °C, respectively. The reuse experiments indicated that the recycled catalysts still maintained excellent activity and stability even after four-time recycling. The present study thus highlights a new approach for the resource utilization of electroplating sludge, which also supplies low-cost and efficient catalytic materials for the selective upgrading of various biomass-derived platform molecules.

研究领域: 催化 · 化学工程 · 环境科学 · 材料科学
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NEW JOURNAL OF CHEMISTRY · 2019 ·Vol. 43 ·期 43 ·16981-16989 · IF 3.069

Ti functionalized hierarchical-pore UiO-66(Zr/Ti) catalyst for the transesterification of phenyl acetate and dimethyl carbonate

Bingying Jia,Miaojiang Wu,Hua Zhang,Yi Zeng,Gongying Wang

Titanates are frequently used as precursors to prepare transesterification catalysts with TiIV species. Unfortunately, it is challenging to control the dispersity of TiIV active sites on supports. Herein, a series of TiIV species is anchored on abundant linker vacancy sites by introducing point and large scale defects in UiO-66(Zr/Ti) with hierarchical-pore structure. The catalyst functionalized by titanium(IV) oxide bis(2,4-pentanedionate) shows excellent catalytic performance in the transesterification of dimethyl carbonate with phenyl acetate. The catalysts are characterized by XRD, FT-IR, N2 adsorption–desorption, XPS, SEM and STEM-HAADF techniques. The results demonstrate that the delicate mesopores in the support can not only exhibit a large surface area for the distribution of the active sites, but also provide better mass transfer performance. Meanwhile, the introduction of octahedral TiIV ions raises the activity of the catalyst via more coordinatively unsaturated ZrIV sites. Furthermore, using titanium(IV) oxide bis(2,4-pentanedionate) as a Ti source can effectively prevent the condensation of tetrahedral TiIV species anchored on the hierarchical-pore UiO-66(Zr/Ti) support.

研究领域: 催化 · 材料科学 · 化学工程
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FUEL · 2022 · IF 8.035

Conversion of glucose into 5-hydroxymethylfurfural catalyzed by Cr-and Fe-containing mixed-metal metal–organic frameworks

Chenxi Lu,Yuanzhuo Zhou,Liangzhi Li,Hongwei Chen,Lishi Yan

Catalytic production of 5-hydroxymethylfurfural (5-HMF) from glucose is a promising routine for generation of varied value-added chemicals. Herein, Mixed-Metal metal–organic frameworks (MOFs)–Fe/MIL-101(Cr) and MIL-101(Cr, Fe) obtained from post-synthesis modification and one-pot synthesis approach respectively were applied for catalytic converting glucose to 5-HMF. The synthesized Mixed-Metal MOFs were characterized by PXRD, SEM, N 2 adsorption–desorption analysis, TGA, XPS and NH 3 -TPD. Cr-and Fe-containing Mixed-Metal MOFs Fe/MIL-101(Cr) and MIL-101(Cr, Fe) presented synergistic effect with enhanced catalytic ability for glucose transformation to 5-HMF compared with typical single-metal MOFs and sulfonic acid-functionalized MOFs. Moreover, these two Mixed-Metal MOFs also presented better thermal stability than single-metal MOFs like MIL-101(Cr). Fe/MIL-101(Cr) was found to possess higher catalytic performance than MIL-101(Cr, Fe). 55.8 % 5-HMF yield was obtained with Fe/MIL-101(Cr) at 170 °C for 2 h in DMSO/water system. In addition, Fe/MIL-101(Cr) demonstrated desired recyclability for five times without incredible loss in its activity. This study provides a Mixed-Metal strategy on MOFs for improving catalytic efficiency of glucose conversion to 5-HMF.

研究领域: 化学工程 · 材料科学 · 催化
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JOURNAL OF MEMBRANE SCIENCE · 2017 · IF 6.035

Fabrication of novel hierarchical ZSM-5 zeolite membranes with tunable mesopores for ultrafiltration

Li Peng,Xiaohan Xu,Xun Yao,Hua Liu,Xuehong Gu

A series of novel hierarchical ZSM-5 zeolite membranes with tunable mesopore sizes have been prepared successfully by using amphiphilic organosilane 3-[(trimethoxysilyl) propyl]octyldimethyl-ammonium chloride (TPOAC) as the mesogenous template and part of the Si source. The effects of several synthesis parameters, such as the TPOAC/SiO 2 ratio, synthesis temperature and crystallization time, on the microstructures and rejection performance of the hierarchical ZSM-5 zeolite membranes were systematically investigated. Multiple techniques, such as XRD , SEM, N 2 adsorption techniques, TEM, IR, 13 C MAS NMR and 29 Si MAS NMR were employed for the characterizations. The filtration of dextran in water shows that the membranes have molecular weight cutoff (MWCO) ranging from 9500 to 943,000, corresponding to the molecular size in the range of 4.5–37   nm. The sharp increase in the rejection of dextran with the increase of molecular weight indicated narrow pore size distribution of the membrane. These results show that the hierarchical mesoporous ZSM-5 zeolite membranes have a great potential for ultrafiltration with high performance.

研究领域: 材料科学 · 化学工程 · 膜技术
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