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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

High-enthalpy biphasic phase change organogels with shape memory function based on hydrophobic association and H-bonding interaction

Chenxiao Yin,Zhi-Xiong Fei,Jingrui Sun,Lin Weng,Xu Wang,Ke-Ke Yang,Ling-Ying Shi

Low-temperature solid–liquid organic phase change materials (OPCMs) offer tremendous opportunities in thermal management techniques but suffer from leakage problems above the melting temperature. Here, inspired with the universal hydro/organogels using three-dimensional polymer networks capable of holding large amounts of liquid solvents, a kind of form-stable high-enthalpy biphasic phase change organogels (BPCOGs) were developed by the integration of hydrophobic association for synthesizing intrinsic phase change matrices and H-bonding interaction for binding OPCM liquids. The porous phase separated poly(acrylamide-octadecyl acrylate) (P(AM- co -OA)) matrices with uniformly dispersed thermal conductive carbon nanotubes were fabricated from the hydrophobically associating hydrogels (HAHs), in which POA segments provide the phase change energy storage microdomains and the PAM network is capable of binding a series of melted OPCMs by hydrogen bond engineering. The fabricated BPCOGs possess form-stability, high phase change enthalpy (high up to 215.5 J g −1 ) and high energy storage efficiency (>90%), and show excellent electrical/optical-thermal energy conversion as well as shape memory performances. This study provides a universal strategy to prepare flexible biphasic OPCMs suitable for a variety of solid–liquid OPCMs including fatty alcohols, fatty acids and polyethylene glycol, and demonstrates the great potentials of these BPCOGs in solar energy utilization and functional flexible devices.

CAS / MDL: 110-18-9
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Advanced Science · 2023 ·Vol. 10 ·期 32 ·2302618 · IF 15.1

Low-Cost Preparation of High-Performance Na-B-H-S Electrolyte for All-Solid-State Sodium-Ion Batteries

Wei Zhou,Changsheng Song,Shuyang Li,Miao Liu,Huiwen He,Shaoyu Yang,Jin Xie,Fei Wang,Fang Fang,Dalin Sun,Jie Zhao,Yun Song

All-solid-state sodium-ion batteries have the potential to improve safety and mitigate the cost bottlenecks of the current lithium-ion battery system if a high-performance electrolyte with cost advantages can be easily synthesized. In this study, a one-step dehydrogenation-assisted strategy to synthesize the novel thio-borohydride (Na-B-H-S) electrolyte is proposed, in which both raw material cost and preparation temperature are significantly reduced. By using sodium borohydride (NaBH 4 ) instead of B as a starting material, B atoms can be readily released from NaBH 4 with much less energy and thus became more available to generate thio-borohydride. The synthesized Na-B-H-S (NaBH 4 /Na-B-S) electrolyte exhibits excellent compatibility with current cathode materials, including FeF 3 (1.0–4.5 V), Na 3 V 2 (PO 4 ) 3 (2.0–4.0 V), and S (1.2–2.8 V). This novel Na-B-H-S electrolyte will take a place in mainstream electrolytes because of its advantages in preparation, cost, and compatibility with various cathode materials.

CAS / MDL: 16940-66-2
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING · 2023 · IF 8.7

Super-flexible and highly conductive H-Ti3C2Tx MXene composite films with 3D macro-assemblies for electromagnetic interference shielding

Xiao-Ai Ye,Si-Ying Zhang,Da-Qiang Zhao,Ling Ding,Kan Fang,Xu Zhou,Gui-Gen Wang

2D MXene are showing great prospects for EMI shielding by virtue of abundant surface functional groups and outstanding metallic electrical conductivity . However, it remains a great challenge to simultaneously achieve flexible, lightweight and high stability in MXene shielding materials due to inferior mechanical strength and poor oxidation stability. Gelation paves up an effective and facile strategy to develop highly stable and conductive 3D porous Ti 3 C 2 T x architectures. Herein, super-flexible and highly conductive H-Ti 3 C 2 T x MXene composite films with 3D macro-assemblies for EMI shielding were fabricated through a gelation-densification process initiated by hydrochloric acids, and two-step vacuum-assisted filtration followed by freeze-casting approach. The obtained nanocomposite films manifest satisfactory mechanical properties with a tensile strength of 116.51 MPa, excellent EMI SE of 55.14 dB, superior SSE/t and high EMI SE retention after 5000 cycles of bending deformation. In addition, the as-prepared nanocomposite papers demonstrate outstanding thermal management performances such as rapid response time, high Joule heating temperature (118 °C) at low applied voltage (2.5 V) and eminent working stability (4000 s).

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APPLIED CLAY SCIENCE · 2021 · IF 5.467

Rapid direct synthesis of nano-H-ZSM-5 from leached illite via solid-like-state conversion-based crystallization

Xinyu Li,Shunyu Han,Dongdong Guan,Nanzhe Jiang,Jingzhe Xu,Sang-Eon Park

The direct synthesis of H-ZSM-5 catalysts from natural aluminosilicate clays is important for the conversion of raw clay resources to high-value-added products. Herein, the solid-like-state conversion was used to directly prepare nano-H-ZSM-5 with uniform morphology and particle size (~300 nm) from leached illite (ISR) as both Si and Al source. Crystallization kinetics indicated that the reactivity of ISR is similar to that of commercially fabricated products and ISR could be rapidly (within 5 h) converted into nano-H-ZSM-5, the crystallinity , morphology, and crystal size of which were strongly affected by the amount of tetrapropylammonium hydroxide (TPAOH). Additionally, the residual Al of ISR uniformly intruded the H-ZSM-5 framework to provide active sites for the methanol-to-aromatics reaction. The catalytic performance stability and BTX selectivity of nano-H-ZSM-5 for this reaction surpassed those of a commercial ZSM-5 catalyst because of the synergistic effect among the specific surface area and volume of micropores , uniform morphology and particle size, and homogeneously distributed acidic sites. This rapid, efficient, and cleaner synthesis reported herein was shown to have no necessity of ion exchange with ammonium salts, to be H-form of ZSM-5 as well as improve the productivity of HZSM-5 catalysts. And consequently, it is expected to reduce the cost of synthesis and provide an opportunity for the comprehensive development and utilization of illite clay resources.

CAS / MDL: 4499-86-9
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2021 · IF 3.171

Efficient conversion of benzene and syngas to toluene and xylene over ZnO-ZrO2&H-ZSM-5 bifunctional catalysts

Xiao Zhao,Xuan Shi,Zhongshun Chen,Long Xu,Chengyi Dai,Yazhou Zhang,Xinwen Guo,Dongyuan Yang,Xiaoxun Ma

A series of ZnO-ZrO 2 solid solutions with different Zn contents were synthesized by the urea co-precipitation method, which were coupled with H-ZSM-5 zeolite to form bifunctional catalysts. As a new benzene alkylation reagent, syngas was used instead of methanol to realize the efficient conversion of syngas and benzene into toluene and xylene. A suitable ratio of ZnO-ZrO 2 led to the significant improvement in the catalytic performance, and a suitable amount of acid helped to increase the selectivity of toluene/xylene and reduce the selectivity of the by-products ethylbenzene and C 9 + aromatics. The highest benzene conversion of 89.2% and toluene/xylene selectivity of 88.7% were achieved over 10% ZnO-ZrO 2 &H-ZSM-5 (Si/Al = 23) at a pressure of 3 MPa and a temperature of 450 °C. In addition, the effect of the zeolite framework structure on product distribution was examined. Similar to the molecular dynamics of aromatic hydrocarbons , H-ZSM-5 zeolites comprise 10-membered-ring pores, which are beneficial to the activation of benzene; hence, the conversion of benzene is higher. H-ZSM-35 and H-MOR zeolites exhibited small eight-membered-ring channels, which were not conducive to the passage of benzene; hence, the by-product ethylbenzene exhibits a higher selectivity. The distance between the active centers of the bifunctional catalysts was the main factor affecting the catalytic performance, and the powder mixing method was more conducive to the conversion of syngas and benzene.

CAS / MDL: 10196-18-6
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CEMENT AND CONCRETE RESEARCH · 2020 · IF 8.328

Effects of pH on the nano/micro structure of calcium silicate hydrate (C-S-H) under sulfate attack

Xin Liu,Pan Feng,Wei Li,Guoqing Geng,Jiale Huang,Yun Gao,Song Mu,Jinxiang Hong

Calcium silicate hydrate (C-S-H), the most important Portland cement hydration product , determines the mechanical properties and durability of cementitious materials . In marine environment, C-S-H often suffers from sulfate attack – one of the most common and severe degradations for concrete. pH is considered as a critical factor in determining the deterioration behavior of C-S-H during sulfate attack, of which the significance may be overlooked. This study focused on the role of pH on the deterioration of C-S-H in terms of the composition and nano/micro structure under sulfate attack. The results show that lowering pH aggravates the decalcification of C-S-H, whereas a strong alkaline condition is beneficial to increase the resistance to deterioration. An increase in the mean chain length together with the proportion of large pores (>10 nm) is observed when C-S-H is subjected to low-pH sulfate attack (pH = 10–12), resulting in a relatively loose structure. The deep analysis on defective tobermorite model reveals that calcium at the interlayer of C-S-H nanostructure is readily removed under sulfate attack, thereby improving the potential of Si-O-Si groups formation and increases the mean chain length of C-S-H.

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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

High mechanical performance Cu-intercalated layered h-BN/N-doped carbon-nanofiber composite films for selective adsorption desulphurization

Xiao-Lu Sun,Zan Liu,Zhi-Lin Cheng

The Cu-intercalated layered h-BN/N-doped carbon-nanofiber composite films (PAN-Cu/ABN-CNFs) were successfully prepared by the combination of the electrospinning technique and the one-pot carbonization process, using the mixed solution of polyacrylonitrile (PAN) and Cu-intercalated activated boron nitride (Cu/ABN) as carbon precursor. A series of characterizations proved that the PAN-Cu/ABN-CNFs possessed the distinguished merits in the structure and composition, such as the pore feature of the micropore (0.076 cm 3 /g)-mesoporous (0.3582 cm 3 /g) structure, the structure of the exfoliated h-BN nanosheets , the low-coordination high-content N (11.65 at%) and the existence of self-reducing Cu nanoparticles (0.5 at%). For adapting the actual application, the mechanical properties of the PAN-Cu/ABN-CNFs were comprehensively evaluated, showing that the PAN-Cu/ABN-CNFs films had the robust tensile strength and bending properties as well as the desirable wear resistance. Furthermore, the selective adsorption desulphurization of the PAN-Cu/ABN-CNFs were examined by the selective adsorption removal of thiophene (TH) from the simulated oil, indicating that the optimum adsorption capacity of the fresh films was up to 78.38 mg/g in 800 mg/L initial concentration and the adsorption capacity after the four-time regeneration recycling still approached 74.894 mg/g. Finally, the adsorption kinetics , isotherm and thermodynamic studies suggested that the adsorption behavior of TH over the PAN-Cu/ABN-CNFs should be better described by the correlation coefficients of Avrami fractional-order kinetics and Liu isotherm, while the thermodynamic studies showed a favorable exothermic and spontaneous adsorption mechanism.

CAS / MDL: 110-02-1
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Additive Manufacturing · 2021 · IF 10.998

H-bonds and metal-ligand coordination-enabled manufacture of palm oil-based thermoplastic elastomers by photocuring 3D printing

Yuchao Wu,Mingen Fei,Tingting Chen,Chao Li,Tengfei Fu,Renhui Qiu,Wendi Liu

Thermoplastic elastomers exhibit high softness, stretchability, recoverability, and reprocessibility, but their manufacture requires high cost and long processing time. Photocuring 3D printing is a remedial processing method as it enables rapid fabrication at room temperature. However, it is difficult to print thermoplastic elastomers by photocuring 3D printing because the generated linear polymers easily dissolve in liquid precursors during printing. Herein, stretchable, self-healing, and renewable palm oil (PO)-based elastomers were prepared from UV-responsive vinyl PO monomers via photocuring 3D printing. Fast solid-liquid separation was achieved via hydrogen bonds and Zn 2+ -ligand coordination (non-covalent crosslinking) to slow down the dissolution of crosslinked polymers in the monomer liquid . The non-covalent bonds endowed the elastomers with high tensile strength (~4.2 MPa) and elongation at break (~851%). Additionally, the elastomers are mainly prepared from biobased, renewable, and low-cost PO feedstocks . Most importantly, the dual dynamic crosslinked network resulted in superior stress relaxation, shape programming, and self-healing behavior of the elastomers. The method described may enhance the application scope of thermoplastic elastomers and 3D printing.

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Solar RRL · 2021 ·Vol. 5 ·期 12 ·2100559 · IF 8.582

Constructing a Cs3Sb2Br9/g-C3N4 Hybrid for Photocatalytic Aromatic C(sp3)?H Bond Activation

Hong-Hong Zhang,Zi-Chun Zhou,Yu-Jie Dong,Li Zhang,Hong-Yan Chen,Dai-Bin Kuang

Utilizing halide perovskites for photocatalytic aromatic C( sp 3 )  H bond activation remains a great challenge due to the serious recombination of photogenerated charge carriers and slow reaction dynamics of the materials themselves. Herein, a lead-free perovskite-based hybrid of Cs 3 Sb 2 Br 9 /g-C 3 N 4 nanosheet is constructed and applied for photocatalytic aromatic C( sp 3 )  H bond activation, which shows enhanced photocatalytic performance. By introducing ultrathin g-C 3 N 4 nanosheets as the heterogeneous nucleation sites, size-reduced and well-dispersed Cs 3 Sb 2 Br 9 nanocrystals can be obtained. The as-formed close contact and high-quality heterointerface between Cs 3 Sb 2 Br 9 and g-C 3 N 4 provides pathways for fast charge transfer which is beneficial to improve the separation efficiency of photogenerated electron−hole pairs. Under visible light irradiation, the Cs 3 Sb 2 Br 9 /g-C 3 N 4 hybrid photocatalyst can effectively oxidize toluene toward benzaldehyde and benzyl alcohol with a total conversion rate of 8346.8 μmol g −1 h −1 , which is 26.6- and 6.0-fold that of pure g-C 3 N 4 and Cs 3 Sb 2 Br 9 , respectively. This work demonstrates the potential of all-inorganic lead-free halide perovskite-based heterostructures for photocatalytic organic reactions.

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Journal of Materials Chemistry A · 2019 ·Vol. 7 ·期 25 ·15137-15144 · IF 10.733

Proton delivery through a dynamic 3D H-bond network constructed from dense hydroxyls for advanced ion-selective membranes

Lei Hu,Li Gao,Xiaoming Yan,Wenji Zheng,Yan Dai,Ce Hao,Xuemei Wu,Gaohong He

An advanced ion-selective membrane containing a dynamic hydroxyl-based 3D H-bond network is first proposed for improved efficiencies and stability in flow battery applications. The 3D H-bond network structure is constructed by the nanoscale aggregation of hydrophilic dense-hydroxyl side chains anchored to hydrophobic polybenzimidazole. This unique dynamic H-bond network creates proton transport highways as well as vanadium permeation barriers across the membrane, leading to an ultralow vanadium ion permeability (<10−9 cm2 s−1) and remarkably low area resistance (0.32 Ω cm−2). This membrane exhibits high coulombic efficiencies (CE: 98.0–99.2%) and energy efficiencies (EE: 88.9–77.9%) at high current densities (80–200 mA cm−2), together with a long lifetime of over 800 cycles (about 42 days) at 120 mA cm−2 in vanadium flow batteries. The design of dynamic 3D H-bond networks provides a promising strategy for the development of highly ion-selective and stable membranes for flow battery application.

CAS / MDL: 6284-40-8
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2019 · IF 7.149

Cathode-Introduced Atomic H* for Fe(II)-Complex Regeneration to Effective Electro-Fenton Process at a Natural pH

Xiao-Cheng Liu,Wen-Qiang Li,Yi-Ran Wang,Guan-Nan Zhou,Yi-Xuan Wang,Chuan-Shu He,Gong-Ming Wang,Yang Mu

Promotion of iron solubility using ligands is the preliminary step in the homogeneous electro-Fenton (EF) process at a mild pH, but the chelate efficiencies of most organic ligands are unsatisfactory, resulting in insufficient Fe(II) availability. In this study, atomic H* was, for the first time, introduced to the EF process to accelerate the regeneration of the Fe(II)-complex at a mild pH using a Ni-deposited carbon felt (Ni-CF) cathode. The introduction of atomic H* significantly elevated total organic carbon (TOC) abatement of ciprofloxacin (CIP) from 42% (CF) to 81% (Ni-CF) at a natural pH. In the presence of humic acids (HAs), atomic H* introduced via Ni-CF enhanced the CIP degradation rate to 10 times that of the CF at a mild pH. The electron spin resonance (ESR), density functional theory (DFT) calculations, electrochemical characterization, and in situ electrochemical Raman study clearly demonstrated that the atomic H* generated from the Ni-CF cathode was highly efficient at reducing Fe(III)-complexes at a natural pH. Additionally, the Ni-CF could generate atomic H* without significant nickel leaching. Thus, the atomic H* could continuously facilitate iron cycling and, consequently, enhance pollutant mineralization via the homogeneous EF process at a mild pH in an environmentally friendly manner.

CAS / MDL: 101385-69-7 7647-01-0
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JOURNAL OF CATALYSIS · 2019 · IF 7.723

Interface synergy between IrOx and H-ZSM-5 in selective C–O hydrogenolysis of glycerol toward 1,3-propanediol

Xiaoyue Wan,Qi Zhang,Mingming Zhu,Yi Zhao,Yongmei Liu,Chunmei Zhou,Yanhui Yang,Yong Cao

Site-selective deoxygenation of hydroxyl groups represents essential processes to access valuable functionalized bio-based compounds with industrial potential. One of the challenging tasks in this context is to convert biodiesel-derived glycerol in the presence of abundant water directly to 1,3-propanediol (1,3-PDO), a key component of the emerging polymer industry. Herein, a monometallic iridium supported on H-ZSM-5 in the absence of Re oxophilic metal oxides was prepared via grinding-assisted impregnation procedures and attempted as an effective and recyclable catalyst for the aqueous-phase selective hydrogenolysis of glycerol toward 1,3-PDO in the absence of acid additives. The results revealed the necessity to control the Ir domain dispersions, Ir 0 /Ir 3+ ratio and the amounts of overall acid/Brönsted acid sites. Activity depended linearly on the amount of overall and Brönsted acid sites, and 1,3-PDO selectivity increased in the presence of Ir-induced Brönsted acid sites, denoted as Ir-O(H)-H-ZSM-5. We speculate that Ir-O(H)-H-ZSM-5 are generated by the interfacial synergistic interaction between IrO x and H-ZSM-5 through hydrogen spillover and reverse hydrogen spillover according to the reported literatures. The reaction mechanism to elucidate the role of Ir-O(H)-H-ZSM-5 sites in glycerol hydrogenolysis was also postulated based on extensive characterization and catalytic reaction results.

CAS / MDL: 16940-92-4
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