ENVIRONMENTAL TECHNOLOGY
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2022
·
IF 3.475
Zhen-xing Yang,Wen-yu Xie,Fang-fang Ye,De-hao Li
Electro-catalytic technology is a promising approach for wastewater treatment, owing to its easy operation, minimal generation of secondary pollution, small foot-print and rapid start-up. In this work, the chlorine evolution potential of the Pd-Sn modified ruthenium(Ru)-iridium(Ir) electrode was investigated for the electro-catalytic treatment of high chlorine ammonia-nitrogen wastewater. The effect of reaction conditions on the removal of ammonia-nitrogen, kinetics and apparent activation energy of ammonia-nitrogen removal were studied. The possible denitrification process of high chlorine ammonia-nitrogen wastewater was discussed. The results indicated that the chlorine evolution potential of the Pd-Sn modified Ru-Ir electrode was 1.0956 V(vs. SCE). The electro-catalytic treatment of high chlorine ammonia-nitrogen conformed to zero-order kinetic law, and the apparent activation energy of removal process was 14.089 kJ/mol. With a current was 0.5 A, the removal efficiency of ammonia-nitrogen could achieve 100% at a reaction time of 40 min. Indirect oxidation played an essential role in the electro-catalytic ammonia-nitrogen removal using the Pd-Sn modified Ru-Ir electrode. This paper demonstrated that the electro-catalytic technology was a promising approach for efficiently treating the high chlorine ammonia-nitrogen wastewater.
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PubMed
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2022
·
IF 3.898
Yachen Deng,Shifu Wang,Yanqiang Huang,Xuning Li
MOF-based materials have been widely explored in electrochemical CO 2 reduction reactions for the production of valuable chemicals. Understanding the reconstruction of those catalysts under working conditions is crucial for the identification of active sites and clarification of reaction mechanism. Herein, a series of six N coordinated Sn-based metal-organic frameworks (Sn-N6-MOFs) are newly developed for electrochemical CO 2 reduction (CO 2 RR). 2% Sn-N6-MOF achieves the optimal catalytic performance with a formate Faradaic efficiency of ∼85% and a current density of 23 mA·cm −2 at −1.23 V vs. RHE. In-situ Raman results combined with ex-situ 119 Sn Mössbauer measurements reveal the structural reconstruction of Sn-N6-MOFs during CO 2 RR, generating tin nanoclusters as the real active sites for CO 2 electroreduction to HCOOH.
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Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 24
·5186-5194
·
IF 6.569
Yan Zhang,Yanjie Liang,Shihai Miao,Dongxun Chen,Shao Yan,Jingwei Liu
A series of Cr3+-doped BaMSi3O9 (M = Zr, Sn, Hf) near-infrared emitting phosphors with tunable luminescence properties have been successfully synthesized by using a simple solid-state reaction method. The developed BaMSi3O9:Cr3+ phosphors show a broad near-infrared emission band ranging from 650 nm to 1200 nm with a peak wavelength longer than 800 nm and a full width at half maximum (FWHM) of more than 155 nm upon blue light excitation. The optimized phosphor also demonstrates good thermal stability, whose emission intensity at 150 °C can retain about 59% of its initial intensity at room temperature. The near-infrared LED prototypes constructed by combining the BaMSi3O9:Cr3+ phosphor with a blue LED chip give a maximum output power of 12.19 mW at a drive current of 320 mA. By using the fabricated near-infrared LED device as a lighting source, night-vision lighting and blood vessel imaging of human fingers and arms are successfully realized, demonstrating the great potential of BaMSi3O9:Cr3+ phosphors for near-infrared LED applications.
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Jingran Xiao,Borui Du,SiYuan Hu,Jun Zhong,Xingyu Chen,Yanghong Zhang,Dongren Cai,Shu-Feng Zhou,Guowu Zhan
It is well-known that sluggish surface charge transfer on a cocatalyst-free hematite photoanode limits its solar conversion efficiency in photoelectrochemical (PEC) water splitting. Here, Mo is used as a codopant synergistically with Sn in α-Fe2O3 to solve this problem. Besides causing a slight narrowing of bandgap, morphological change, and even sublimation loss of α-Fe2O3, Mo doping also imports low-valent Fe due to charge compensation with MoV/VI as indicated by X-ray photoelectron spectroscopy and Bader charge computation, which increases the densities of donor and surfaces states. Although rate law analysis demonstrates slight retardation of surface reaction kinetics, strongly inhibited charge recombination in surface states by Mo doping still contributes to improving the photocurrent density and reducing the onset potential of α-Fe2O3 and Sn–Fe2O3 photoanodes. An optimized Mo/Sn–Fe2O3 photoanode can realize a low onset potential of 0.68 V vs a reversible hydrogen electrode (VRHE) and a photocurrent density of 1.97 mA cm–2 at 1.23 VRHE, enhanced by 58% and 20 times compared to Sn–Fe2O3 and α-Fe2O3, respectively. It is demonstrated that Mo doping promotes charge transfer which differs from most traditional n-type dopants that facilitate charge separation but inhibit charge transfer. This report expands the n-type dopant family of α-Fe2O3 for efficient PEC water splitting.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Xiangbo Song,Jun Yue,Yuting Zhu,Chengyan Wen,Lungang Chen,Qiying Liu,Longlong Ma,Chenguang Wang
Efficient and one-pot conversion of biomass-derived carbohydrate into highly value-added 5-hydroxymethylfurfural (HMF) is a crucial reaction step for the valorization of biomass resources toward bio-based chemicals and fuels. In this work, a series of Sn/SAPO-34 catalysts were prepared through impregnation and evaluated in glucose conversion to HMF. The physicochemical properties of Sn/SAPO-34 catalysts were systematically characterized by SEM, XRD, N2 physisorption, XPS, solid-state 119Sn, 29Si, and 31P NMR, XRF, UV–vis, NH3-TPD, and pyridine-FTIR techniques. It was demonstrated that controlling the Sn loading amount could facilely adjust the acid strength and acid amount of the SAPO-34 zeolite. The incorporation of Sn species could induce the formation of a tetrahedrally coordinated Sn4+ site and Sn-OH site to improve the amounts of Brønsted and Lewis acid sites of the catalyst. However, modification with sufficiently high Sn loading could decrease the acid strength and performance of the catalyst owing to its structure damage. The 5%Sn/SAPO-34 catalyst (i.e., Sn loading calculated based on the mass ratio of SnCl4·5H2O as a precursor to the parent SAPO-34) was found to exhibit the superior catalytic performance under mild conditions and could afford an HMF yield of 64.4% at 98.5% glucose conversion in a biphasic 35 wt % NaCl-H2O/tetrahydrofuran (THF) system at 150 °C within 1.5 h. Additionally, a catalytic reaction pathway was proposed, involving the adsorption of glucose molecules by the −Cl group on the catalyst via a hydrogen bond, followed by glucose isomerization to fructose over the Lewis acid Sn4+ and Al3+ sites and, finally, fructose dehydration to HMF catalyzed by the Brønsted acid Sn-OH and Si-OH-Al sites. The activity of the catalyst decreased due to the leaching of the active site Sn after several consecutive cycles. This work provides insights into the improvement in the Sn-containing zeolite catalyst for tandem conversion of glucose to HMF.
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MATERIALS CHEMISTRY AND PHYSICS
·
2021
·
IF 4.094
Shengqiang Zhou,Lipeng Zhou,Yunlai Su,Xiaomei Yang,Hao He
Sn-Beta zeolite is a promising heterogeneous Lewis acid catalyst. Hydrothermal synthesis of Sn-Beta(TEOS) using tetraethyl orthosilicate (TEOS) as silica source is a classical method. However, the hydrolysis of TEOS generates considerable ethanol, which is unfavorable for scalable production of Sn-Beta. Herein, cheap fumed silica and silica sol were used as Si sources to synthesize Sn-Beta and compared with that synthesized from TEOS . The crystalline phase, morphology, physicochemical properties, and the state of Sn were characterized. It was found that Sn-Beta can be successfully prepared with fumed silica and silica sol as well as TEOS as silica source. Sn was introduced into the framework of these samples. Sn-Beta synthesized from fumed silica (Sn-Beta(FS)) and silica sol (Sn-Beta(Sol)) had similar crystallization behavior and full crystallization time as well as morphology, crystal size with that from TEOS. Sn-Beta(Sol) has less silanols and lowest ratio of open/closed tin site among these samples. It exhibited higher catalytic activity for the conversion of glucose to methyl lactate and lower catalytic activity for the isomerization of glucose as compared with the other two samples. Sn-Beta(FS) showed similar catalytic performance in the studied reactions with Sn-Beta(TEOS).
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2020
·Vol. 45
·期 4
·6273-6284
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IF 3.741
Xiaolin Shao,Qi Zhang,Xurui Zhang,Jin Yi,Yuyu Liu,Jiujun Zhang
Summary A facile method is developed to fabricate nanoporous, structured, Sn-based catalyst electrodes. Sn, Zn, and multiwalled carbon nanotubes (MWCNTs) are co-electrodeposited on a copper substrate, followed by chemical dezincification in NaOH aqueous solution to remove Zn. By controlling variables such as the contents of Zn and MWCNTs, a series of Sn-MWCNT/Cu (S Z MC) electrodes are fabricated. Experimental results show that using such novel S Z MC electrodes can achieve a HCOO − Faradaic efficiency of over 91% at −0.99 V versus RHE for 10 hours in CO 2 -saturated 0.5 M KHCO 3 aqueous solution. The high performance is attributed to the addition of MWCNTs and Zn, followed by chemical dezincification to remove Zn and then create vacancies in the catalyst structure, which results in a special porous structure of S Z MC with large surface area. Then ECSA is used for enhancing the catalytic activity and selectivity of HCOO − production, as well as promoting intermediate adsorption and mass transfer.
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JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Ying Xu,Tao Yuan,Zihao Bian,Junhe Yang,Shiyou Zheng
Sn is an attractive anodic material for lithium-ion batteries. High-temperature reduction is large-scale technique since most elemental Sn exists in the form of oxides. However, it is still a challenge to fabricate high performance Sn-based anodes with well-dispersed Sn nanoparticles in conductive matrix due to low melting point of Sn and tendency of particle agglomeration . Herein, we systematically investigate the influences of reduction conditions on particle and phase formation of Sn/carbon nanofibers (CNF) from electrospun SnO 2 /polyacrylonitrile. It is shown that the SnO 2 can be reduced to Sn with slight aggregation at low temperature of 500 °C in a reducing atmosphere, but the composites possess poor electronic conductivity . As raising temperature, the grain size of Sn increases accordingly leading to sluggish Li + internal diffusion dynamics. While in an inert atmosphere , the SnO 2 cannot be reduced completely at low temperature until 650 °C. By optimal control, the Sn/CNF–N 2 -700 calcined at 700 °C in N 2 atmosphere presents the best electrochemical Li-ion storage performance among these samples, which delivers a reversible capacity of 932.2 mAh g −1 at 100 mA g −1 and stable cycling life with 760.3 mAh g −1 retention after 200 cycles. This study may provide optimization guidance for industrial manufacture of Sn-based materials.
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JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
Xuelong Zhou,Liyu Lin,Yunhui Lv,Xiangyang Zhang,Liangdong Fan,Qixing Wu
Component materials and flow fields are key design parameters that influence the advection-diffusion-reaction process and thereby the performance of a Sn–Fe hybrid flow battery . In this work, various electrode configurations (empty chamber and porous carbon-based electrodes), membranes (cation and anion conducting) and flow fields (serpentine and interdigitated) are systematically investigated to elucidate their effects on the unique charge/discharge behaviors of the Sn–Fe flow battery with tin metal plating/striping. It is found that the battery capacity roughly increases linearly with the porosity of the porous electrode especially at low current densities , and a highly porous electrode (graphite felt) is more desirable than an empty chamber configuration in terms of capacity and power density. In addition, as compared to cation exchange membrane (Nafion 212), the anion exchange membrane (Fumasep FAP-450) exhibits improved capacities and columbic efficiencies in sulfuric acid-based electrolytes at low current densities due to the reduction of cation crossover. Interestingly, it is showed that although a serpentine flow field and a low flow rate generally lead to poor battery performance, they tend to ameliorate the maldistribution of plated tin at the negative electrode owing to the restricted mass transfer of reactants.
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FUEL
·
2022
·
IF 8.035
Tianliang Lu,Xianfeng You,Yanlong Zong,Yongming Xu,Xiaomei Yang,Lipeng Zhou
Production of γ-valerolactone (GVL) from ethyl levulinate (EL) was studied by catalytic transfer hydrogenation (CTH) strategy under mild conditions. Hydrothermally synthesized Sn-Beta zeolites with high crystallinity show high catalytic activity and selectivity. With isopropanol as hydrogen source, 97.1 % GVL yield with 100 % selectivity was given under 110 °C. Crystallization time for synthesis of Sn-Beta showed great effect on the catalytic performance. Sn-Beta- x d catalysts with longer crystallization time (≥7 days) have high crystallinity and better catalytic performance. Firstly, longer crystallization time is necessary for the formation of large amount of Lewis acid sites which catalyze the conversion of EL to GVL. Secondly, high level of silanol groups in Sn-Beta has negative effect on the catalytic performance. High crystallinity means the amount of silanol groups in Sn-Beta- x d at a low level which is favorable for this CTH reaction. Meanwhile, this is why hydrothermally synthesized Sn-Beta shows higher catalytic activity than post-synthesized Sn-Beta in the conversion of EL to GVL. Furthermore, the catalyst was reusable.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 34
·11904-11912
·
IF 4
Jiaying Yan,Xuanyu Wang,Fanghua Ning,Jin Yi,Yuyu Liu,Kai Wu
Electrochemical reduction of carbon dioxide (CO2ER) has become an effective solution to relieve the energy crisis and tackle climate change. In this study, a series of tin-based organic frameworks modified by In (Sn-MOF/Inx) were successfully synthesized via a simple hydrothermal method and explored for high formate-selective CO2ER. The pure Sn-MOF exhibits maximum formate selectivity with a faradaic efficiency (FEformate) of approximately 85.0% and a current density of 15 mA cm−2 at −1.16 VRHE, while the In (6%)-modified Sn-MOF (Sn-MOF/In6) delivers a much higher maximum FEformate (around 97.5%) and a current density of 16 mA cm−2 at −0.96 VRHE. Remarkably, the Sn-MOF/In6 exhibits a significantly larger specific surface area (183.3 m2 g−1) compared to the Sn-MOF (65.2 m2 g−1). These findings indicate that introducing In, an alien element with a slightly different outer orbital electron number from that of Sn, can significantly boost the selectivity and activity for CO2ER to formate. This study presents an efficient way to modify MOF catalysts through a well-designed introducing process.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 10
·3147-3157
·
IF 5
Hange Wang,Wen Chen,Wei Jin,Yueli Liu
SCR technology is considered to be the most effective method for denitrification. However, the low NOx conversion rate of the current catalysts at low temperatures limits their further application. Herein, Sn-doped modified CoAl-LDH carriers are synthesized by a hydrothermal method, and the typical hexagonal sheet structure of the MnOx(0.25)/CoSn3Al-LDO catalyst achieves 100% NO conversion at a wide range of 120–330 °C with a GHSV of 30 000 h−1, and the 100% NO conversion may be maintained at 200 °C for 30 h. After the introduction of 150 ppm SO2 at 200 °C, the NO conversion of the MnOx(0.25)/CoSn3Al-LDO catalyst is maintained at 73.4%, which is greatly improved compared with those of CoAl-LDO and MnOx(0.25)/CoAL-LDO catalysts (64.8% and 38.6%, respectively). The active components such as MnOx and Co3O4 are highly dispersed in the MnOx(0.25)/CoSn3Al-LDO catalyst. Sn doping increases the ratios of Mn4+/Mn3+ and Co3+/Co2+ as well as the adsorbed oxygen amount on the catalyst surface, and improves the redox capacity of the catalyst and increases the number of acid sites, resulting in the excellent low-temperature NH3-SCR performance of MnOx(0.25)/CoSn3Al-LDO.
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