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可持续化学
Green Energy & Environment · 2019 ·Vol. 4 ·期 4 ·424-431 · IF 0

Highly efficient catalytic valorization of biomass-derived hexoses and furfuryl alcohol in the presence of polymer-based catalysts

Yangyang Zhang,Xinli Tong,Linhao Yu,Lingwu Meng,Pengfei Guo,Song Xue

The catalytic transformation of furfuryl alcohol and hexose into value-added chemicals have been investigated with a series of polymer-based catalysts including poly(styrenesulfonic acid) (PSS), graphite oxide-doped poly(styrenesulfonic acid) (PSS-GO), and graphite-doped poly(styrenesulfonic acid) (PSS-C). It is found that the selective conversion of furfuryl alcohol to methyl levulinate (MLE) was successfully performed with PSS as the catalyst, in which a 96.4% yield is attained in methanol solvent. Moreover, the efficient dehydration of d -fructose to produce 5-hydroxymethylfurfural (HMF) has also been achieved using PSS-GO as the catalyst, where a 76.5% yield of HMF was obtained in N -methylpyrrodinone solvent. The effects of reaction temperature, time and solvent were investigated. Furthermore, the used catalysts have been respectively characterized by XRD, TG, FTIR, SEM and TEM techniques to reveal the physical properties and structures of these polymeric catalytic materials.

研究领域: 催化化学 · 生物质能源 · 绿色化学 · 有机转化 · 高分子材料 · 可持续化学 · 生物基化学品
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FUEL PROCESSING TECHNOLOGY · 2019 · IF 4.507

Metal-organic framework containing Brønsted acidity and Lewis acidity for efficient conversion glucose to levulinic acid

Haonan Qu,Bingyi Liu,Guohua Gao,Yiming Ma,Yanmei Zhou,Hua Zhou,Li Li,Yonghong Li,Shengjian Liu

Levulinic acid (LA) is a versatile key building block in the conversion of carbohydrates and it is an important basic chemical with various potential uses. MIL-100(Fe) loading with insoluble lysine functionalized phosphotungstic acid (Lys-PM 2 ) as heterogeneous catalysts have been synthesized for the conversion of glucose to LA in water. The optimized yield of LA is obtained by using Lys-PM 2 to catalyze glucose conversion is comparable to the majority of effective catalysts. The highest yield of LA (57.9%) is obtained at 150 °C for 9 h with 100 mg glucose and 25 mg Lys-PM 2 , since the Brønsted acidity and Lewis acidity of Lys-PM 2 . And the catalyst is able to recycle at least four times. It demonstrates the potential of Lys-PM 2 for the conversion of biomass.

研究领域: 催化化学 · 绿色化学 · 生物质能源 · 有机转化 · 材料化学 · 可持续化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Formic acid recovery from EDTA wastewater using coupled ozonation and flow-electrode capacitive deionization (Ozo/FCDI): Performance assessment at high cell voltage

Longqian Xu,Yu Xie,Yang Zong,Yunfeng Mao,Bing Zhang,Huaqiang Chu,Deli Wu

Carbon resource recovery from toxic organic wastewater to reduce unnecessary energy loss and greenhouse gas emissions is rarely pursued. In the present study, a promising approach for formic acid (FA) recovery from EDTA wastewater was proposed by coupling ozonation and flow-electrode capacitive deionization (Ozo/FCDI). In the ozonation process, a FA productivity of 25% was obtained with the complete degradation of EDTA. The FA recovery from wastewater was compared under electrodialysis (i.e., without the use of flowable carbon electrodes, 0 wt%) and FCDI (i.e. using 5 wt% flowable carbon electrodes) processes and the results demonstrated the superiority of the FCDI process. After 390 min of operation, the accumulated FA concentration in the anode chamber of the FCDI system had increased to 633.6 mg/L with a low energy consumption of 8.0 kWh/kg FA, which was 1.8 times of the FA concentration in the electrodialysis (ED) process and nearly 6.4 times in the feed stream. These findings suggest the effective acquisition of high value-added FA in the Ozo/FCDI system; may provide new opportunities and challenges for the recovery of organic compounds.

研究领域: 环境工程 · 废水处理 · 资源回收 · 电化学工程 · 可持续化学 · 污染控制化学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2022 · IF 4.598

A green strategy towards fabricating FePO4-graphene oxide for high-performance cathode of lithium/sodium-ion batteries recovered from spent batteries

Shihan Zeng,Qinxin Xu,Hongjun Jin,Lingxing Zeng,Yiyi Wang,Wenbin Lai,Qi Yao,Jixiang Zhang,Qinghua Chen,Qingrong Qian

Owing to the growing concern about the resource shortage and environmental pollution caused by the vast usage of lithium-ion batteries, the recycle of spent lithium-ion power batteries in electric vehicles becomes urgent. Herein, we report a one-pot method to recover FePO 4 from spent LiFePO 4 cathode powder through advanced oxidation , which is further successfully used as cathode materials of lithium/sodium-ion batteries (LIBs/SIBs) for the first time. With this facile method, the electrochemical performance can be further improved by simply optimizing FePO 4 with graphene oxide coating. The optimized FePO 4 -graphene oxide (FePO 4 -GO) exhibits enhanced electrochemical performances of 145 mAh g −1 at 0.5 C for LIBs and 75 mAh g −1 at 0.1 C for SIBs , as well as high capacity retention (144 mAh g −1 at 1 C after 300 cycles for LIBs ; 61 mAh g −1 at 1 C after 300 cycles for SIBs). We expect that our current work will provide a facile and green strategy to recover LiFePO 4 material from spent batteries.

研究领域: 材料科学 · 储能 · 电化学 · 可持续化学 · 电池技术
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS · 2022 · IF 6.437

Facile synthesis of multifunctional poly(ionic liquid)s as an advanced three-way catalyst for the efficient production of lignite-derived arenes

Zhong-Qiu Liu,Guo-Qiang Zhang,Xin Huang,Yuan-Yuan Yu,Yu-Jing Liu,Anguo Ying

The precise synthesis of multifunctional poly(ionic liquid)s (MFPILs) featuring basic sites, mesoporous channels, and hydrophobicity continues to be a substantial challenge. Moreover, the directional conversion of lignite to monocyclic arenes (MCAs) is highly attractive but particularly challenging on account of its geometrical complexity and chemical inertness. The efficiency of lignite directional conversion to MCAs over solid bases is substantially decreased by the presence of water molecules leading to the deactivation and leaching of basic sites. Herein, the novel solid bases, i.e. , MFPILs with dibasic sites, unique hydrophobicity , and abundant mesoporous channels, were successfully fabricated by a radical multicomponent cross-linked copolymerization for the first time. Even more excitedly, the resulting MFPILs were demonstrated to be very efficient for directional catalytic hydroconversion of extraction residue from Dahuangshan lignite (DL ER ) into MCAs with 32.3 wt% yield, which is by far the highest value reported for lignite-derived MCAs by solid bases under similar conditions. The synergistic catalysis, i.e. , hydrophobic microenvironment, mesoporous confinement, and synergistic effect of dibasic sites, for active hydrogen transfer of DL ER conversion into MCAs over MFPILs is confirmed by characterization methods. The work not merely sheds substantial light on developing the novel solid bases, but also exhibits a potentially powerful catalyzing strategy to synthesize MCAs.

研究领域: 催化化学 · 高分子化学 · 能源材料 · 可持续化学 · 有机转化
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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Reaction milling for scalable synthesis of N, P-codoped covalent organic polymers for metal-free bifunctional electrocatalysts

Xinxin Lin,Peng Peng,Jianing Guo,Zhonghua Xiang

This study exploits an effective mechanochemical process (termed as reaction milling) to conduct Schiff-based coupling reaction with melamine and terephthalaldehyde for the synthesis of covalent organic polymer (RM-COP) as the carbon skeleton and the derivative phosphorus doped material (RM-COP-PA). Comparing with the tradition solvothermal method with reaction time of 3 days under 120 °C, the newly developed reaction milling method significantly shorten the reaction time of the synthesis to 3 h under room temperature as well as bypassing the usage for hazardous solvents. The space-time yield of the developed reaction milling method for synthesis of the bifunctional electrocatalytic precursor reaches 189 kg m −3  day −1 . Significantly, the optimal products followed by further carbonization (RM-COP-PA-900) demonstrated excellent bifunctional electrocatalytic activities for an efficient ORR performance with similar commercialized Pt/C half-potential of 841 mV vs RHE as well as an IrO 2 -like OER activity with a potential of 1.69 V at 10 mA cm −2 in alkaline media, which is better than most metal-free bifunctional catalysts. Moreover, the obtained RM-COP-PA-900 exhibits much better durability and resistance to crossover effect even than the commercial 20 wt% Pt/C catalysts. Therefore, this work will open up a rapid, solvent-free and scalable approach for, but not limit to, highly efficient electrocatalysts.

研究领域: 材料科学 · 电化学 · 可持续化学 · 能源材料 · 纳米技术
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ACS Omega · 2022 · IF 4.132

Biomass Hierarchical Porous Carbonized Typha angustifolia Prepared by Green Pore-Making Technology for Energy Storage

Shuya Wang,Yidong Mei,Zishuo Shao,Jingru Wang,Zhenzhen Tan,Zurui Qiu,Minghao Wang,Hong Zheng

The cost-effective biomass-derived carbon with high electrochemical performance is highly desirable for the sustainable development of advanced energy storage devices. In this manuscript, Typha angustifolia with a large output and loose porous characteristics was selected as the raw material of biomass. In the synthesis process, KHCO3, which is more environmentally friendly, is used as a pore-forming agent, and the low-cost, easy-to-clean fluxing agent NaCl is used to assist the pore-forming process. Based on the analysis of thermogravimetric-infrared test results, the calcination procedure of porous carbon was designed reasonably, so that the functions of the pore-forming agent and fluxing agent could be fully exerted. Its high electrochemical performance is attributed to combined contributions from high surface area and hierarchical porous structures. The as-prepared carbon also showed an outstanding capacitance of 317.2 F/g at a current density of 1 A g–1 and a high capacitance retention of over 97.83% after 5000 cycles at a current density of 4 A g–1. This work provides an outstanding renewable candidate and a feasible route design strategy for the fabrication of high-performance electrodes.

研究领域: 材料科学 · 能量存储 · 可持续化学 · 纳米技术 · 电化学
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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

Solvent-Free Crystallization of Zeolitic Imidazolate Framework Membrane via Layer-by-Layer Deposition

Pingping Yang,Zhan Li,Zhuangzhuang Gao,Mingqiu Song,Jinya Zhou,Qianrong Fang,Ming Xue,Shilun Qiu

Searching for sustainable synthesis methods of metal–organic framework (MOF) membranes has received huge attention in both academia and industry. In this contribution, the compact ZIF-8 membrane with excellent gas separation performance was successfully prepared via an environmentally friendly and simple method, in which the artful layer-by-layer deposition approach was used to achieve the solvent-free crystallization of a well-intergrown and defect-free ZIF-8 membrane. The solvent-free process is a simple and generalized method for construction of MOF membranes, which can avoid using solvents and high autogenous pressure and brings great benefits for energy saving, emission reduction, and safety as well as scalable manufacturing. In addition, the solvent-free crystallization of MOF membranes exhibits more unprecedented advantages to fill the common intercrystalline cracks, pinhole defects, and grain boundary defects on the membrane. The resulting thin ZIF-8 membrane exhibited both competitive H2 permeability of 6.7 × 10–7 mol m–2 s–1 Pa–1 and high H2/CO2 selectivity of 12.3, simultaneously, which is one of the best ZIF-8 membranes ever reported.

研究领域: 材料科学 · 膜技术 · 可持续化学 · 分离科学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2022 · IF 5.518

Green preparation of N-doped hierarchical porous carbon composites from humic acid extraction residue of lignite as anodes for lithium/sodium-ion batteries

Hai-Bang Zhang,Zexu Yang,Kaiyuan Qiao,Guixiao Jia,Huazheng Sai,Yunying Liu,Wenxiu He,Jin-Long Cui

Heteroatom doping is a valid strategy for improving the lithium/sodium storage capacity of carbon materials. Here, N-doped hierarchical porous carbon (NHPC) with defects is designed and synthesized via a low-cost and green synthesis method using lignite humic acid extraction residue as the raw material. Through experiments and theoretical calculations, the effects of N-doping and defects on Li + /Na + storage capacity are systematically analyzed. With the introduction of defects and N atoms, electrical conductivity , and Na + adsorption energy of NHPC gain improvement. The porous structure could shorten the Li + /Na + diffusion path and relieve the volume dilation and mechanical strain. Compared with other counterparts, NHPC obtained at 700 °C maintains a bigger reversible capacity of 940 mAh/g at 0.1 A/g in lithium-ion batteries. Even at 1.0 A/g, the specific capacity of NHPC-700 stabilizes at 508 mAh/g with a capacity recession of only 0.021% per cycle after 1000 cycles. In sodium-ion batteries, NHPC-700 anode also exhibits a high specific capacity (320 mAh/g at 0.1 A/g) and good cycling stability (225 mAh/g after 1200 cycles at 1.0 A/g). Here, the entire synthesis route is an eco-friendly process, which achieves zero discharge and zero pollution.

研究领域: 材料科学 · 储能技术 · 电化学 · 可持续化学 · 纳米材料
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RARE METALS · 2020 ·Vol. 39 ·期 9 ·1099-1106 · IF 2.161

Clean utilization of palm kernel shell: sustainable and naturally heteroatom-doped porous activated carbon for lithium–sulfur batteries

Han Xu-Ran,Guo Xiao-Tian,Xu Meng-Jiao,Pang Huan,Ma Yan-Wen

Lithium–sulfur batteries (LSBs) have received much concern as emerging high-power energy storage system. Nevertheless, the low conductivity of sulfur and polysulfide shuttle results in low rate capability and rapid capacity decay, which seriously limit its commercial application. Here, facile, sustainable and cost-effective strategy for preparing heteroatom-doped porous activated carbon (PAC) derived from biomass palm kernel shell (PKS) was developed for high-performance LSB applications. The presence of N, P and S heteroatoms with modification of the surface polarity brings about large amounts of active sites and improved adsorption property compared to those of common carbon materials. The PAC sample possesses desirable specific surface area (SSA) (2760 m 2 ·g −1 ) as well as pore volume (1.6 cm 3 ·g −1 ). Besides, the good electrical conductivity of PAC endows the material with excellent rate performance. The PAC-S electrode with a 60% of sulfur loading has a desirable first discharge capacity (1045 mAh·g 1 , 200 mA·g −1 ) with superb discharge capacity (869.8 mAh·g −1 , 100th cycle) and cyclability (312.6 mAh·g −1 , 800 mA·g −1 , 1000th cycle), which can be mainly ascribed to its unique porous properties and the good conductivity of PAC. Graphic abstract

研究领域: 能源材料 · 电化学 · 可持续化学 · 电池技术 · 纳米多孔材料
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DALTON TRANSACTIONS · 2012 ·Vol. 41 ·期 41 ·12915-12919 · IF 3.838

Ionothermal synthesis of two open-framework zirconium phosphates and their gas adsorption properties

Wei Wang,Lei Liu,Jiangfeng Yang,Sanying Li,Jinping Li,Jinxiang Dong

From a deep eutectic mixture consisting of trimethylammonium chloride (TMACl) and oxalic acid, two templated zirconium phosphates, ZrPOF-TMA1 with 8- and 10-ring pore channels as well as ZrPOF-TMA2 with 7- and 8-ring pore channels, have been synthesized. A low P/Zr ratio is necessary for ZrPOF-TMA1, and higher P/Zr ratios tend to form ZrPOF-TMA2, but the former cannot be obtained by templating TMACl under hydrothermal conditions. This is the first example in which a trimethylammonium cation, a protonated tertiary amine, has been used as a template to successfully synthesize two microporous zirconium phosphate materials, showing the potential for novel chemistry in ionothermal reactions. Both materials have a relatively high thermal stability and are stable up to 410 °C. Of the two microporous materials, ZrPOF-TMA2 with small pore openings exhibits a highly effective pore-selective behaviour that can discriminate between CO2 and CH4, with a CO2/CH4 adsorption ratio of 12.7 at 1 bar.

研究领域: 材料化学 · 无机化学 · 气体分离 · 多孔材料 · 可持续化学
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RSC Advances · 2019 ·Vol. 9 ·期 53 ·30815-30822 · IF 3.049

A biobased Schiff base from protocatechualdehyde and its application in flame-retardant, low-smoke epoxy resin systems

Weiqi Xie,Shiwen Huang,Shumei Liu,Jianqing Zhao

Herein, a new renewable Schiff base flame retardant 4,4′-((1E,1′E)-((oxybis(4,1-phenylene))bis(azanylylidene))bis(methanylylidene))bis(benzene-1,2-diol) (PH-ODA) was prepared by the reaction of protocatechualdehyde with 4,4′-diaminodiphenyl ether (ODA). PH-ODA (acting as a carbonization agent) combined with ammonium polyphosphate (APP) were used as intumescent flame retardants for commercial bisphenol A epoxy resin (DGEBA). For the cured epoxy resin containing 7.5% APP and 2.5% PH-ODA, the limiting oxygen index (LOI) reached 29.9% (with the V-0 rating in UL-94 test), and the peak heat release rate and total smoke production were respectively decreased by 88.1% and 68.3%, compared with pure epoxy resin. The enhancement of fire-safety performance was due to PH-ODA/APP promoting the formation of a compact intumescent char structure. It was also found that the synergism between PH-ODA and APP was helpful to enhance the fire resistance of the epoxy matrix. This work provides a facile and sustainable route for synthesizing Schiff base compounds from biomass-derived resources, possessing great potential for application in highly-effective intumescent flame retardants.

研究领域: 高分子科学 · 材料化学 · 火灾安全工程 · 可持续化学 · 阻燃材料
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