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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Natural DNA-derived highly-graphitic N, P, S-tridoped carbon nanosheets for multiple electrocatalytic applications

Qian Yu,Jingshu Wang,Haibo Li,Ruiqing Li,Suyuan Zeng,Rui Li,Qingxia Yao,Hongyan Chen,Konggang Qu,Yao Zheng

In the electrocatalytic oxygen reduction and hydrogen evolution reactions (ORR/HER), metal-free carbon-based materials presented great potentials as alternatives to Pt because of their flexible adjustability of electronic and geometric properties. The pursuit of high-performance carbons demand for high-level doping, large surface area and high graphitization, but the improvement of the former two aspects would inevitably impair the third one, which seems a contradictive proposition. Herein, by a facile “mix-and-pyrolyze” method, natural DNA was first developed to synthesize N, P, S-tridoped carbons (NPSC) with porous sheet structures, high graphitization, large surface areas and abundant high-quality dopants simultaneously. Thus, the newly-prepared NPSC displays superior alkaline ORR performance comparable to Pt/C together with excellent acidic activity and better stability. Meanwhile, NPSC is one of most active acidic HER catalysts and the best alkaline HER catalyst among carbon counterparts. Density function theory computation reveled the origins of superior performance are attributed to positively charged C sites neighboring to S for ORR and P sites for HER because of DNA-derived advantaged structural features. The as-fabricated rechargeable zinc–air battery based on current tridoped carbon has closed peak power density and specific capacity but much better charge–discharge stability compared with Pt/C.

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ACS Omega · 2024 · IF 3.7

Selective N═S Coupling Reactions of N-Methoxy Arylamides and Sulfoxides Catalyzed by Iron Salt

Dandan Jiang,Yingzhen Zhang,Xin Qiao,Jun Xiao,Kunming Liu,Juanhua Li,Jinbiao Liu

An iron-catalyzed selective N═S coupling of N-methoxy amides and sulfoxides has been developed and was found to be a highly efficient method for the synthesis of N-acyl sulfoximines. Electron-donating as well as electron-withdrawing groups on the phenyl ring are tolerated, and even sensitive substituents are compatible. The current catalytic transformation was conducted under an air atmosphere and can be easily scaled up to a gram scale with a catalyst loading of only 1 mol %. In this case, both coupling partners are used in their native forms, thus obviating prior functionalization and activation.

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CRYSTENGCOMM · 2019 ·Vol. 21 ·期 40 ·6010-6017 · IF 3.382

Study on growth characteristics of Ib-type diamond in an Fe–Ni–C–S system

Shuai Fang,Hongan Ma,Zhanke Wang,Zhiqiang Yang,Zheng-hao Cai,Luyao Ding,Xinyuan Miao,Liangchao Chen,XiaoPeng Jia

FeS is the main sulfur-containing compound in natural diamond inclusions. The research on FeS-doped diamond crystals plays an extremely important role in exploring the growth environment of natural diamond and the chemical composition of the earth. In our work, the characteristics of FeS doped diamond crystals were studied by using a China-type large volume cubic high-pressure apparatus with an iron–nickel alloy as a catalyst at 6.0 GPa and 1300–1350 °C. The crystals were characterized by OM, SEM, XPS, FTIR and Raman. Scanning electron microscopy of the crystal shows that the {100} plane of the crystal is rougher than {111}, which is related to the number of dangling bonds on different crystal faces of the crystal. The residue on the surface of the crystal was detected by mapping, and the test result showed that it was a sulfur iron and a sulfur nickel compound. FeS will decompose in the synthesis system, and the decomposition products are Fe and S2.The XPS spectrum of the crystal shows that S was successfully incorporated into the diamond lattice by forming C–S–O and C–S–SO2–C bonds, and the peak intensity was strong. The infrared spectrum shows that the N content in the crystal gradually increases as the doping ratio increases. Raman spectroscopy analysis shows that the S-doped Ib-type diamond single crystal has a high-quality sp3 structure, and the full width at half maximum (FWHM) of the crystal gradually broadens as the doping ratio increases.

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JOURNAL OF APPLIED ELECTROCHEMISTRY · 2016 ·Vol. 46 ·期 7 ·725-733 · IF 2.223

Enhanced electrochemical performance from cross-linked polymeric network as binder for Li–S battery cathodes

Zhu Shaoyin,Yu Jiaojiao,Yan Xiao,Zhao Erqing,Wang Yanqing,Sun Deye,Jin Yongcheng,Kanamura Kiyoshi

Abstract A sulfur cathode with enhanced electrochemical properties is prepared by a hydrogel binder owning three-dimensional polymeric network for Li–S batteries. The promising high-performance binder (Alg-Ca 2+ ) is constructed by an in situ interconnection of alginate chains by additive divalent cation with a facile and self-assembly strategy. With the assistance of 3D network, the sulfur/activated carbon composite cathode exhibits a higher rate capability and cycling performance compared to poly(vinylidene fluoride) binder, and the capacity retention is up to 80.6 % after 200 cycles (0.5C, 1C = 1675 mA g −1 ). Additionally, the electrochemical impedance spectroscopy also reveals a lower electrode resistance and better kinetic characteristics with Alg-Ca 2+ as a binder. The improved electrochemical behaviors are assigned to the ability of maintaining the electrode stability due to the excellent mechanical property and amorphous structure. Graphical Abstract

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JOURNAL OF POLYMER RESEARCH · 2012 ·Vol. 19 ·期 10 ·1-12 · IF 1.733

Sulfonated copoly(norbornene)s bearing sultone pendant groups and application as proton exchange membranes candidates

Hu Meiping,He Xiaohui,Chen Yiwang,Chen Defu

Novel copolynorbornenes bearing pendant sultone groups (designated as P(BN/SulNBOH) and P(BN/SulNBOMe)) have been successfully synthesized via copolymerization of functionalized norbornenes bearing sultones (designated as SulNBOH and SulNBOMe) with 2-butoxymethylene norbornene (BN). The catalyst system showed high catalyst activity (10 4 g polymer /mol Ni ·h) and the obtained copolymers have high molecular weight and a narrow molecular weight distribution. Furthermore, the achieved copolymers P(BN/SulNBOH) and P(BN/SulNBOMe) were converted into sulfonated copolymers sP(BN/NBOH) and sP(BN/NBOMe). Both sP(BN/NBOH) and sP(BN/NBOMe) membranes displayed low water uptake, high thermal properties, good mechanical properties, and better proton exchange membranes properties. The proton conductivities measured in the hydrated state at 80 °C ranged from 10 −5 to 7.19 × 10 −3  S·cm −1 . Novel copolynorbornenes bearing pendant sultone groups are synthesized. The achieved copolymers are converted into the sulfonated copolymers. The proton conductivities of the membranes measured in the hydrated state at 80 °C ranged from 10 −5 to 7.19 × 10 -3  S·cm −1 .

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Journal of Cleaner Production · 2021 · IF 9.297

S-doped carbon nanosheets supported ZnO with enhanced visible-light photocatalytic performance for pollutants degradation

Yin Zhang,Guomin Zhao,Lu Gan,Hailan Lian,Mingzhu Pan

The exploration of highly efficient and stable visible-light-driven photocatalysts remains a great challenge for organic pollutant management. Herein, a novel S-doped carbon nanosheet (SCN)/ZnO composite photocatalyst has been synthesized via a facile method using the freeze-drying cellulose nanocrystals (CNCs) as the carbon precursor. The surface morphology and chemical environment of SCNs can be regulated simultaneously with S-doping. Compared to the pristine carbonized CNCs (CN), the SCN carbonized at 550 °C (SCN-550) has regular nanosheet-like morphology, integrated graphitic structures ( I D / I G of 0.692), rich surface heteroatoms (14.62 at% for O, 1.93 at% for S), and most content of oxidized-S atoms (100 at%). It endows the increased surface reactive sites (specific surface area of 45.55 m 2  g −1 ), accelerated electron transfer , enhanced visible-light absorption, and prolonged carrier lifetime for the corresponding SCN-550/ZnO composite. Consequently, the SCN-550/ZnO shows an outstanding photocatalytic performance for methylene blue (99%). In addition, SCN-550/ZnO composite exhibits general application to organic contaminants , including phenol (91%), formaldehyde (92%), acetone (79%), and methyl alcohol (84%), respectively. Furthermore, the strong interaction of Zn–O–C covalent bond between SCN-550 and ZnO ensures the high photocatalytic activity of SCN-550/ZnO composite after four cycles, demonstrating its excellent reusability and stability. This study develops a highly efficient visible-light photocatalyst of CNCs derived S-doped carbon nanosheets supported ZnO for environment purification.

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Polymers · 2021 ·Vol. 13 ·期 20 ·3489 · IF 4.329

Crosslinked Fluorinated Poly(arylene ether)s with POSS: Synthesis and Conversion to High-Performance Polymers

Yashu He,Jingting Wang,Igor S. Sirotin,Vyacheslav V. Kireev,Jianxin Mu

This study reports on a series of crosslinked poly(arylene ether)s with POSS in the main chain. The fluorinated and terminated poly(arylene ether)s were first synthesized by the nucleophilic reaction of diphenol POSS and decafluorodiphenyl monomers, including decafluorobiphenyl, decaflurobenzophenone, and decafluorodiphenyl sulfone. They were then reacted with 3-hydroxyphenyl acetylene to produce phenylacetylene-terminated poly(arylene ether)s. The polymers were of excellent processability. When heated to a high temperature, the polymers converted into a crosslinked network, exhibiting a low range of dielectric constant from 2.17 to 2.58 at 1 HMz, strong resistance against chemical solutions, low dielectric losses, and good thermal and hydrophobic properties.

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JOURNAL OF POLYMER SCIENCE · 2023 ·Vol. 61 ·期 6 ·472-481 · IF 3.4

Synthesis of precision poly(1,3-bicyclo[1.1.1]pentane alkylene)s via acyclic diene metathesis polymerization

Xiang-Yue Cheng,Fu-Sheng Du,Zi-Chen Li

1,3-Disubstituted bicyclo[1.1.1]pentane (BCP) is a rigid, linear, non-conjugated hydrocarbon unit that is usually transformed from [1.1.1]propellane. This unit has been introduced into drugs as mimics of 1,4-disubstituted benzene moieties and used as rigid linkers in small-molecule materials. However, the influence of this unique structure on the polymer properties has only been scarcely investigated. In this work, three symmetrical α,ω -diene monomers containing one and two BCP units were synthesized for the first time from [1.1.1]propellane. Three types of precise poly(1,3-bicyclo[1.1.1]pentane alkylene)s with BCPs located on every 11th and 21st chain carbons were obtained via acyclic diene metathesis (ADMET) polymerization and subsequent hydrogenation. All these polymers show higher thermal stability than linear polyethylene. For polymers containing one BCP moiety in their repeating unit, BCP acts as a defect to distort the PE crystals and decrease the melting temperature of PE. However, the polymer that containing a [2]staffane moiety (two jointed BCP units) in the polymer backbone forms a new crystalline morphology. This work elucidates the impact of BCP units on the thermal and crystallization behavior of PE, providing new insights of utilizing BCP unit to construct new polymer backbone, regulate the packing order of polymers and their properties. Graphical

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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Scalable 3D Honeycombed Co3O4 Modified Separators as Polysulfides Barriers for High-Performance Li–S Batteries

Liping Wu,Chuyue Cai,Xi Yu,Zihe Chen,Yuxin Hu,Fang Yu,Shengjun Zhai,Tao Mei,Li Yu,Xianbao Wang

Lithium sulfur batteries (LSBs) are regarded as one of the most promising energy storage devices due to the high theoretical capacity and energy density. However, the shuttling lithium polysulfides (LiPSs) from the cathode and the growing lithium dendrites on the anode limit the practical application of LSBs. To overcome these challenges, a novel three-dimensional (3D) honeycombed architecture consisting of a local interconnected Co3O4 successfully assembled into a scalable modified layer through mutual support, which is coated on commercial separators for high-performance LSBs. On the basis of the 3D honeycombed architecture, the modified separators not only suppress effectively the “shuttle effects” but also allow for fast lithium-ions transportation. Moreover, the theoretical calculations results exhibit that the collaboration of the exposed (111) and (220) crystal planes of Co3O4 is able to effectively anchor LiPSs. As expected, LSBs with 3D honeycombed Co3O4 modified separators present a reversible specific capacity with 1007 mAh g–1 over 100 cycles at 0.1 C. More importantly, a high reversible capacity of 808 mAh g–1 over 300 cycles even at 1 C is also acquired with the modified separators. Therefore, this proposed strategy of 3D honeycombed architecture Co3O4 modified separators will give a new route to rationally devise durable and efficient LSBs.

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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Two dimensional sulfonated molybdenum disulfide (S–MoS2) thin-film nanocomposite nanofiltration membrane for selective desalination

Jinyuan Zhu,Wenqiao Meng,Qiang Xue,Kaisong Zhang

Nano-fillers will be an attractive strategy to improve salt fractionation of nanofiltration (NF) membrane if the integrity problem of nano-fillers in PA layer is well addressed. In this work, molybdenum disulfide (MoS 2 ) nanosheets sulfonated with 1,3-propane sultone was added to the aqueous phase to participate in the interfacial polymerization reaction and construct a novel thin-film nanocomposite (TFN) nanofiltration membrane . A series of characterization and discussion were carried out on the obtained nanomaterials and membranes. The S–MoS 2 nanosheet can be well wrapped by the resulted PA layer, thereby preserving the integrity of the PA skin. Furthermore, The TFN membranes possessed enhanced electronegativity and hydrophilicity and the PA layer became thinner and denser after introducing the sulfonated MoS 2 nanosheets (S–MoS 2 ) in the PA matrix. In particular, the optimal S–MoS 2 composite membrane exhibits excellent performance, which approximately reach 99% divalent salt (Na 2 SO 4 ) rejection and 1.4-fold water permeance of the pristine membrane. Overall, this study provided a novel way for separation treatment of hypersaline wastewater.

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MACROMOLECULES · 2022 · IF 6.057

Thermoresponsive Properties of Poly[oligo(ethylene glycol) sorbate]s Prepared by Organocatalyzed Group Transfer Polymerization

Yujian Liu,Yongyao Lei,Yougen Chen

The current contribution presents the synthesis of poly[oligo(ethylene glycol) sorbate]s (PREGmSs) by the t-Bu-P4-catalyzed group transfer polymerization (GTP) method, their postpolymerization modification at the backbone double bond, and thermoresponsive properties in aqueous solution. Four oligo(ethylene glycol) sorbate monomers (REGmSs), including 2-(2-methoxyethoxy)ethyl sorbate (MeEG2S), 2-(2-(2-methoxyethoxy)ethoxy)ethyl sorbate (MeEG3S), 2-(2-(2-ethoxyethoxy)ethoxy)ethyl sorbate (EtEG3S), and 2-(2-(2-(2-methoxyethoxy)ethoxy)ethoxy)ethyl sorbate (MeEG4S), are newly designed to study the thermoresponsive properties of their related polymers. The t-Bu-P4-catalyzed GTP of REGmS only proceeds in a 1,4-regioselective addition manner to quantitatively produce the backbone trans-rich (ca. 80%) PREGmS. The complete hydrogenation and epoxidation of the backbone double bonds result in hydrogenated and epoxidized polymers (PREGmS-H2 and PREGmS-epoxy, respectively), which have different main-chain structures and rigidity from their parent PREGmS. Given the 1,4-substituted structure of a sorbate monomer, the chemical structure determination of PREGmS-H2 by 13C NMR spectra demonstrates that the above polymers have an erythro-rich (ca. 60%) structure in diastereochemistry and a diisotactic/disyndiotactic ratio around 1:1 in stereoregularity. The thermoresponsive properties of PREGmS, PREGmS-H2, and PREGmS-epoxy in aqueous solutions are studied in detail from various aspects in terms of polymer mass concentration, molecular weight, length and end group of the oligo(ethylene glycol) side chain, and main-chain structure by turbidity, 1H NMR spectroscopy, and dynamic light scattering (DLS) methods, which are discussed below.

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Materials Today Energy · 2020 · IF 5.604

Ag/polypyrrole co-modified poly(ionic liquid)s hydrogels as efficient solar generators for desalination

Chaohu Xiao,Weidong Liang,Qi-Meige Hasi,Lihua Chen,Jingxian He,Fang Liu,Chengjun Wang,Hanxue Sun,Zhaoqi Zhu,An Li

Solar steam generation is one of the most promising technologies to utilize solar energy, which is applied to extract fresh water from seawater or contaminated water. However, solar vapour generation is usually restricted to the underutilization of solar energy or depends on complicated light-harvesting adjuncts. Here, a novel hierarchically double-layered evaporation device was demonstrated based on poly(ionic liquid)s hydrogel with the upper surface co-modified by polypyrrole (PPy) and silver particles (named as Ag/PPy-PMBA-BrILs). The evaporation system exhibits a cooperative interaction of the double-layer with efficient light-absorbing and water transportation, leading to a high evaporation rate of 1.37 kg m −2  h −1 with a photothermal conversion efficiency of 88.7% under 1 sun illumination. The high evaporation rate is mainly due to the synergistic light absorption of polypyrrole and silver particles as well as the excellent water transfer capability of poly(ionic liquid)s hydrogel. Moreover, the hydrogel-based evaporation device also exhibits excellent salt-resistant performance for solar desilination in artificial sea water. The high-efficiency poly(ionic liquid)s hydrogel based solar steam generator with co-modified light-absorbing surface may open new opportunities for the future design and fabrication of high-performanced solar steam generator for practical applications.

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