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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Small molecule DOPO-p-DP crosslinked 6FDA-DAM-Br-85% carbon molecular sieve membrane with superior aging for efficient gas separation

Xiuling Chen,Lei Wu,Cong Xie,Shan Xu,Yanfang Fan,Nanwen Li

Carbon molecular sieve (CMS), as the gas separation membrane materials, still faces challenges for regulation pore diameter precisely. In this work, we propose to reconstruct the 6FDA-DAM-Br-85% polyimide CMS membranes by introducing 6,6'-(1,4-phenylenebis(((4-hydroxyphenyl)amino)methylene))bis(dibenzo[c,e][1,2] oxaphosphinine6-oxide) small molecule compound (DOPO- p -DP) as crosslinking agent to regulate the pore distribution. The crosslinked precursors were obtained via the reaction between C–Br bond in 6FDA-DAM-Br-85% polyimide and N–H bond in DOPO- p -DP compound, the precursors and CMS membranes (550 °C- 2 h) were characterized with ATR-TFIR, XRD and XPS. The pore size distribution of crosslinked CMS membranes was range in 4.5–8.0 Å from the N 2 adsorption data. The crosslinked CMS membranes exhibited excellent gas separation performance, which was strongly dependent on the mass fraction of DOPO- p -DP, an increasing mass fraction of DOPO- p -DP leaded to improve in gas selectivity, while reduced its permeability. The 6FDA-DAM-Br-85%/DOPO- p -DP-20% CMS membrane showed the impressive permeability and superior gas selectivity, the permeabilities of O 2 , CO 2 , and H 2 are 798, 3018, and 13560 Barrer combined with the O 2 /N 2 , CO 2 /CH 4 , and H 2 /CH 4 selectivities of 7.8, 65.6, and 294.8 respectively, the separation performances surpassed the latest trade-off relationship. In addition, the 20% of the DOPO- p -DP crosslinked CMS membrane revealed the superior aging behaviour than that of the 6FDA-DAM-Br-85% CMS membrane over 480 h aging under vacuum conditions.

✓ 已验证 DOI 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

MOF-derived CuCo carbon microspheres assembled with nitrogen-doped carbon nanotubes as PMS activator for the efficient degradation of p-nitrophenol

Qingqing Shi,Yaqi Hou,Qiting Zhu,Yongmei Hao

Due to the complex structure of metal–carbon-based catalysts derived from metal-organic frameworks (MOFs), it is difficult to clarify the active sites and catalytic mechanisms. Constructing of structure–activity relationship is conducive for identifying active center, but there is still a gap in the bimetal-carbon-based catalysts/PMS systems. Here, we report a highly efficient and stable CuCo bimetal-nitrogen doped carbon catalyst (CuCo@C-N) for the activation of PMS for efficient degradation of PNP. By manipulating the catalyst structure, establishing the structure–activity relationship and combining with DFT calculation, the non-metallic active centers were determined, including defects, C=O and graphite N. Co was the only metal active center, and the presence of Cu accelerated the redox cycle of the system. The degradation of PNP was dependent on electron transfer and ROS activation. The metal active center was used to generate sulfate radicals (SO 4 •− ), and the non-metal active sites accelerated electron transfer and non-radical pathways to generate 1 O 2 .

✓ 已验证 DOI 高影响因子
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2018 · IF 2.88

A simple yet sensitive colorimetric nitrite ions assay based on diazotization with p‑Aminobenzoic and coupling with phloroglucinol in acidic medium

Mohammed Hassan Ibrahim,Zhonghua Xue,Mahgoub Ibrahim Shinger,Hassan Idris Abdu,Lulu Xiong,Duoliang Shan,Xiaoquan Lu

Immoderate intake of nitrite (NO 2 − ) is deleterious human health and may result in causing dangerous diseases. In this study, nitrite detection system was successfully fabricated based on a unique diazo-coupling reaction of p‑Aminobenzoic acid (PABA) and phloroglucinol (1, 3, 5‑trihydroxybenzene). Upon the presence of NO 2 − in an acid medium, p‑Aminobenzoic acid could not only form diazonium ion easily but also couple with p‑Aminobenzoic acid, and results forming yellow water-soluble azo dye that shows maximum absorption at 434 nm. Under the further accurate determination condition, such as acid concentration, amount of reagents and time required, the naked-eye detection of NO 2 − showed excellent selectivity in compared with some anions. Especially, diazotization and coupling reaction proposed here is very fast and control of pH and temperature are unnecessary. Moreover, the color is stable for several days and Beer's law is obeyed over a wide range. Reliable detection can be made in the range of 0.05 to 1 p.p.m. of nitrite ion. Detection limit was calculated to be 0.024 p.p.m. (0.52 μ M) by UV–visible spectroscopy and 0.05 p.p.m. (1.09 μ M) by naked-eye. By using an electrochemical method, IR, SEM, and 1 HNMR, the sensing mechanism can be easily verified. More importantly the proposed method was successfully applied for the determination of nitrite in a real water sample.

✓ 已验证 DOI 高影响因子
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CHEMISTRY-A EUROPEAN JOURNAL · 2022 ·Vol. 28 ·期 71 ·e202202410 · IF 5.02

The Core/Shell Structure P Doped MoS2@Ni3S2 Nanorods Array for High Current Density Hydrogen Evolution in Alkaline and Acidic Electrolyte

Yong Gao,Dani Zhang,Jingjing Li,Hao Gong,Cheng Jiang,Hairong Xue,Xianli Huang,Tao Wang,Jianping He

Graphical The P doped MoS 2 @Ni 3 S 2 nanorods array with core/shell structure was prepared through successive sulfuration and phosphorization strategies, which exhibits close catalytic activity to Pt/C, the overpotential is only 290 mV at 250 mA cm −2 . Electrocatalysis is the most promising strategy to generate clean energy H 2 , and the development of catalysts with excellent hydrogen evolution reaction (HER) performance at high current density that can resist strong alkaline and acidic electrolyte environment is of great significance for practical industrial application. Therefore, a P doped MoS 2 @Ni 3 S 2 nanorods array (named P-NiMoS) was successfully synthesized through successive sulfuration and phosphorization. P-NiMoS presents a core/shell structure with a heterojunction between MoS 2 (shell) and Ni 3 S 2 (core). Furthermore, the doping of P modulates the electronic structure of the P-NiMoS; the electrons transfer from the t 2g orbital of Ni element to the e g empty orbital of Mo element through the Ni−S−Mo bond at the Ni 3 S 2 and MoS 2 heterojunction, facilitating the hydrogen evolution reaction. As a result, P-NiMoS exhibits excellent HER activity; the overpotential is 290 mV at high current density of 250 mA cm −2 in alkaline electrolyte, which is close to Pt/C (282 mV@250 mA cm −2 ), and P-NiMoS can stably evolve hydrogen for 48 h.

✓ 已验证 DOI 高影响因子
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ORGANIC ELECTRONICS · 2020 · IF 3.31

Efficient and stable mesoporous perovskite solar cells using p-type poly (9-vinylcarbazole) modified the interface of perovskite/mesoporous TiO2 layers

Jiaji Duan,Yuning Liu,Xiaohong Chen,Sumei Huang,Wei Ou-Yang,Guang Zhu,Sanjun Zhang,Zhuo Sun

A p-type poly(9-vinylcarbazole) (PVC) was inserted into the interface between perovskite and mesoporous TiO 2 electron transport layers. The ultrathin PVC modified TiO 2 layer can obviously improve the crystallinity of perovskite layer with less pinholes, passivate the interface and inhibit hole carriers transport into the interface of perovskite/TiO 2 electron transport layers. The perovskite film modified with PVC shows larger grain sizes and more compact films, which helps to increase photocurrent and reduce the leak current of cells. The passivating interface with less hole carrier accumulation and hydrophobicity can greatly reduce carrier recombination, improve carrier transport and extraction abilities and cells stability. Therefore, perovskite solar cells (PSCs) with PVC modified TiO 2 layer exhibited a power conversion efficiency (PCE) of 19.02%, which is remarkably higher than that (16.09%) of the reference cells. Furthermore, PSCs without and with PVC modification respectively retained 20% and 55% of the initial PCE values aging for 30 days at the relative humidity 15% in air without encapsulation. For thermal stability test, the pervoskite layers were heated for 10 h at 100 °C before further spin-coating Spiro-OMeTAD, PSCs with PVC modification were still remained 70% of the original PCEs, which is greatly higher than that (30%) of the reference cells. These results indicate that PSCs with PVC modified TiO 2 layer can effectively improve PCEs and show better moisture resistance and thermal stability.

✓ 已验证 DOI 高影响因子
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INORGANICA CHIMICA ACTA · 2021 · IF 2.545

The difference of uranyl (UO22+) complexes with Nitrilotri–3–propanoic acid and Tris(2–carboxyethyl) phosphine: N–tricarboxylate versus P–tricarboxylate

Xingliang Li,Juncai Lu,Wanjun Mu,Baihua Chen,Daibing Luo,Bijun Liu,Yanqiu Yang,Hongyuan Wei,Shuming Peng

Nitrilotri–3–propanoic Acid (NTPA) and Tris(2–carboxyethyl) phosphine (TCEP) possess similar skeleton. This pair of isostructural ligands is a perfect set to assess the differences of uranyl (UO 2 2+ ) complexes with N–tricarboxylate versus P–tricarboxylate. The protonation reactions of NTPA and TCEP were investigated by potentiometry and calorimetry. Complexation of uranyl with the both ligands was studied by potentiometry and structural analysis. The results indicate that central trialkylamine in NTPA has a higher affinity for the proton than trialkylphosphine in TCEP. Crystal structures and NMR analyses indicate that central amine of NTPA and central phosphine of TCEP are not involved in the bonding. NTPA/UO 2 2+ complex is more stable than TCEP/UO 2 2+ complex. This difference cannot be explained by electronic effect of central N and P atoms because of nonbonding interactions. The higher stability of UO 2 2+ /NTPA versus UO 2 2+ /TCEP may be due to the fact that the central N atom of NTPA has a lower steric hindrance than the central P atom of TCEP. Another possible reason is that UO 2 2+ /TCEP complexes have different coordination modes from UO 2 2+ /NTPA complexes.

✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Cobalt anchored on porous N, P, S-doping core-shell with generating/activating dual reaction sites in heterogeneous electro-Fenton process

Huajing Zhou,Huichang Dong,Jinghao Wang,Yuancai Chen

A novel controllable mesoporous core–shell microsphere (Co/Fe 3 O 4 @PZS) is synthesized by polycondensation, and used as ORR electrocatalyst in the heterogeneous electro-Fenton (hetero-EF) reaction. Characteristic analysis indicated that PZS offered massive reactive sites for anchoring Co ions on the shell. Heteroatom Lewis acidic active sites, related with pyridinic N (4.15%), P = N/P-N (6.46%) and S = O (3.19%) bonds, were formed through the replacement of C = C groups with the N-P-S doped at the shell, which benefited the activating/generating reactive oxygen species (ROS), and capturing/degrading the target pollutant substrates. Moreover, PZS shells prevent the nano-Fe 3 O 4 crystals in the core from direct contact with the solution, which would greatly improve the stability of electrode with almost no leaching of Fe/Co ions after six successive runs. Electrochemical experiments confirmed the accelerating electron transfers among ≡Fe II/III /≡Co II/III by the direct electric activation, as evidenced by the decreasing potential discrepancy (from 0.175 to 0.123 V) and sharply increasing ring current (from 35 to 200μA), markedly improved the ORR toward two-electron process (n = 2.01). ESR and radical scavenging experiments verified that •OH and 1 O 2 served as the main ROS in the Co/Fe 3 O 4 @PZS hetero-EF system. In addition to the two-electron reduction ( O 2 → H 2 O 2 → Â · O H ), O 2 could also be directly electro-activated to 1 O 2 via one-electron reduction ( O 2 → Â · O 2 - / Â · HO 2 - → 1 O 2 ). Additionally, the regenerating/reducing of ≡Fe III /Co III could get the electron directly from the cathode without excess consumption of H 2 O 2 , all these could eventually facilitate BPA degradation with lower energy consumption (1.318 kWh m −3 ). This study provides a reliable and facile route to prepare mesoporous core–shell microsphere, and developed as doped cathode in the field of electro-Fenton electrocatalysis process.

✓ 已验证 DOI 高影响因子
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2014 · IF 2.93

Fabrication of highly dispersed palladium/graphene oxide nanocomposites and their catalytic properties for efficient hydrogenation of p-nitrophenol and hydrogen generation

Weining Sun,Xiaofeng Lu,Yan Tong,Zhen Zhang,Junyu Lei,Guangdi Nie,Ce Wang

In this report, graphene oxide (GO) nanosheets decorated with ultrafine Pd nanoparticles (Pd NPs) have been successfully fabricated through a reaction between [Pd 2 (μ-CO) 2 Cl 4 ] 2− and water in the presence of GO nanosheets without any surfactant or other reductant . The as-synthesized small Pd NPs with average diameter of about 4.4 nm were well-dispersed on the surface of GO nanosheets . The Pd/GO nanocomposites show remarkable catalytic activity toward the hydrogenation of p -nitrophenol at room temperature . The kinetic apparent rate constant ( k app ) could reach about 34.3 × 10 −3  s −1 . Furthermore, the as-prepared Pd/GO nanocomposites could also be used as an efficient and stable catalyst for hydrogen production from hydrolytic dehydrogenation of ammonia borane (AB). The catalytic activity is much higher than the conventional Pd/C catalysts.

✓ 已验证 DOI 高影响因子
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES · 2023 ·Vol. 39 ·期 4 ·690-696 · IF 3.1

Heavy Rare Earth Element Gd Enhancing Thermoelectric Performance in p-Type Polycrystalline SnSe via Optimizing Carrier Transport and Density of States

Xu Pengfei,Hua Yezhen,Jin Kangpeng,Xu Biao

Tin selenide(SnSe) material exhibits very excellent thermoelectric properties in both p- and n-type single crystals, benefiting from advantageous electronic structure and ultra-low lattice thermal conductivity. However, poor mechanical properties and time-consuming production limit its practical application, and polycrystalline SnSe has attracted great attention in recent years. Herein, the SnSe microplates are prepared by a facile solvothermal method and compacted by spark plasma sintering (SPS). With enhanced electrical conductivity( σ ) and optimized Seebeck coefficient( S ) benefited from the Sn vacancies and increased density of states effective mass by the incorporating of heavy rare earth element Gd, an enhanced power factor(PF) value of about 0.86 mW/(m·K 2 ) is realized in the p-type polycrystalline Sn 0.985 Gd 0.015 Se sample. Combined with the medium total thermal conductivity k tot and lattice thermal conductivity k lat of 0.7 and 0.56 W/(m·K), respectively, an enhanced peak dimensionless figure of merit( ZT ) of ca. 1.1 was achieved at 873 K along vertical to the SPS pressing direction. The average ZT was also improved as compared to that of the pristine SnSe sample.

✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Heteroatom doping-induced Pt dispersion and electronic effect for boosting the catalytic performance in the hydrogenation of nitrobenzene to p-aminophenol

Chong Yao,Jiwei Wu,Limei Pan,Lu Yu,Jie Luo,Jinjin Shan,Jie Liu,Chunshan Lu,Feng Feng,Xiaoliang Xu,Lili Lin,Yuxue Yue,Qingtao Wang,Jia Zhao,Qunfeng Zhang,Xiaonian Li

N-doped carbon materials were synthesized using a straightforward salt template method for Pt metal modification, resulting in a reduction in particle size from 4.8 nm to 2.1 nm due to the interaction between Pt and the carrier. The hydrogenation activity of nitrobenzene increased by 4.5 times compared to undoped catalysts. Additionally, the electronic effects of N and Pt enhanced the selectivity of p-aminophenol by up to 20.4 %. The anchoring of Pt by N improved the stability of active metal centers in a strong acidic system, thereby retarding Pt loss. Theoretical calculations and characterization revealed that the enhancement of activity relied on the high dispersion of Pt, while the improvement in product selectivity was associated with changes in the adsorption strength of the phenylhydroxylamine intermediate. N anchoring of Pt, inducing an electron effect, disentangled the activity and selectivity of nitrobenzene hydrogenation for the preparation of p-aminophenol.

✓ 已验证 DOI 高影响因子
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JOURNAL OF APPLIED POLYMER SCIENCE · 2021 ·Vol. 139 ·期 16 ·51987 · IF 3.125

Improving the mechanical performance of P(N-hydroxymethyl acrylamide/acrylic acid/2-acrylamido-2-methylpropanesulfonic acid) hydrogel via hydrophobic modified nanosilica

Pan Xu,Yi Zong,Zhijie Shang,Meiling Yao,Pingde Liu,Xinxue Li

Hydrogels with high mechanical strength are essential for its most industrial applications. In this work, the hydrophobic SiO 2 nanoparticles (M-SiO 2 NPs) modified with octadecyltrimethoxysilane were used as physical crosslinker to toughen the mechanical properties of hydrogels. The solution of monomers containing M-SiO 2 NPs, N-hydroxymethyl acrylamide (NHAM), acrylic acid (AA), 2-acrylamido-2-methylpropanesulfonic acid (AMPS), was polymerized to prepare a P(NHAM/AA/AMPS)-based composite hydrogel without any chemical cross-linker. The composition and microstructure of the hydrogel were carefully studied with Fourier transform infrared spectroscopy and scanning electron microscopy. The mechanical properties of the hydrogel were investigated through compressive and tensile tests. Dynamic swelling tests were carried out at different pH values (1.0–12.0) and salinity (2000–20,000 mg/L) to study the acid resistance, alkali resistance, and salt resistance of the hydrogel. The obtained results showed that the hydrogel exhibited excellent mechanical performance, which was attributed to the unique 3D network formed by the hydrogen bond between M-SiO 2 NPs and polymer as well as the hydrophobic association effect between the hydrophobic chains of M-SiO 2 NPs. Furthermore, the hydrophobic association effect was enhanced when contacting with salt, acid, and alkali solutions, thus endowing the hydrogel with intensified salt resistance and wider acid–base adaptability range.

✓ 已验证 DOI 高影响因子
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ELECTROCHIMICA ACTA · 2019 · IF 5.383

Three-dimensional P-doped carbon skeleton with built-in Ni2P nanospheres as efficient polysulfides barrier for high-performance lithium-sulfur batteries

Zhaoxu Guang,Ying Huang,Xuefang Chen,Xu Sun,Mingyue Wang,Xuansheng Feng,Chen Chen,Xudong Liu

Rational design of modified separator is of great significance in effectively suppressing the shuttle of lithium polysulfides (LiPSs) and hence realizing fulfilling cycling performance of lithium-sulfur batteries (LSBs). In this paper, we developed a facile strategy to fabricate P-doped carbon coated CNT skeleton coupled with nickel phosphide (Ni 2 P) nanospheres (PCCNT@NPS), and then we employed the as-developed hybrid as a multifunctional modified interlayer onto PP separator (denoted as PCNPmPP) to face the challenge of LiPSs shuttling. The as-prepared hybrid provides abundant physical confinement and strong chemical adsorption for inhibiting polysulfides shuttling as well as efficient catalysis for accelerating LiPSs converting. As a result, the LSBs based on PCCNT@NPS modified PP separator have delivered a highly reversible cycling performance with high initial discharge capacity of 1067 mAh g −1 and low capacity decay rate of 0.077% per cycle within 500 cycles at 1 C. The promising results demonstrate that the PCCNT@NPS composite is capable of effectively inhibiting the diffusion and shuttle of LiPSs. This paper provides a novel thinking for the synthesis of multifunctional interlayer onto PP separator for advanced LSBs.

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