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NEW JOURNAL OF CHEMISTRY · 2017 ·Vol. 41 ·期 19 ·10613-10618 · IF 3.269

One-pot synthesis of N-substituted pyrroles from nitro compounds and 2,5-hexadione over a heterogeneous cobalt catalyst

Zheng Gong,Yu Lei,Peng Zhou,Zehui Zhang

In this study, the one-pot heterocyclization of nitro compounds with 2,5-hexadione was studied for the synthesis of N-substituted pyrroles via a Paal–Knorr condensation process. The heterogeneous cobalt–nitrogen catalyst (Co–Nx/C-800-AT) was found to be active for this reaction with formic acid. Formic acid served as a hydrogen donor for the transfer hydrogenation, and also acted as an acid catalyst. More importantly, this method was tolerant of other functional groups, and hence various N-substituted pyrroles were produced with good to excellent yields. The Co–Nx/C-800-AT catalyst was highly stable, and could be reused several times without loss of its catalytic activity.

研究领域: 有机化学 · 催化化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF ORGANIC CHEMISTRY · 2024 · IF 3.3

Controlled and Site-Selective C–H/N–H Alkenylation, Dialkenylation, and Dehydrogenative β-Alkenylation of Various N-Heterocycles

Jin Yan,Suijie Zhong,Xu Chen,Yihuan Luo,Hua Cao,Xiang Liu,Limin Zhao

Here, we report controlled and site-selective C–H alkenylation and dialkenylation of indolizines and pyrrolo[1,2-a]quinolines with β-alkoxyvinyl trifluoromethylketones under simple and practical conditions. Moreover, this direct C–H alkenylation strategy can also be extended to imidazo[1,2-a]pyridines. Notably, without a transition metal and external oxidant, efficient dehydrogenative β-alkenylation of tertiary amines with β-alkoxyvinyl trifluoromethylketones is presented.

研究领域: 有机化学 · 合成化学
✓ 已验证 DOI 高影响因子
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Advanced Science · 2024 · IF 14.3

Stretchable, Self-Healing, and Bioactive Hydrogel with High-Functionality N,N′-bis(acryloyl)cystamine Dynamically Bonded Ag@polydopamine Crosslinkers for Wearable Sensors

Wei Shi,Hui Li,Jing Chen,Yern Chee Ching,Cheng Hock Chuah,Chengsheng Xu,Moran Liu,Jinyong Zhang,Kuan Yong Ching,Yongsheng Liang,Guanglin Li,Wei Tang

Hydrogels present attractive opportunities as flexible sensors due to their soft nature and tunable physicochemical properties. Despite significant advances, practical application of hydrogel-based sensor is limited by the lack of general routes to fabricate materials with combination of mechanical, conductive, and biological properties. Here, a multi-functional hydrogel sensor is reported by in situ polymerizing of acrylamide (AM) with N,N′-bis(acryloyl)cystamine (BA) dynamic crosslinked silver-modified polydopamine (PDA) nanoparticles, namely PAM/BA-Ag@PDA. Compared with traditional polyacrylamide (PAM) hydrogel, the BA-Ag@PDA nanoparticles provide both high-functionality crosslinks and multiple interactions within PAM networks, thereby endowing the optimized PAM/BA-Ag@PDA hydrogel with significantly enhanced tensile/compressive strength (349.80 kPa at 383.57% tensile strain, 263.08 kPa at 90% compressive strain), lower hysteresis (5.2%), improved conductivity (2.51 S m −1 ) and excellent near-infrared (NIR) light-triggered self-healing ability. As a strain sensor, the PAM/BA-Ag@PDA hydrogel shows a good sensitivity (gauge factor of 1.86), rapid response time (138 ms), and high stability. Owing to abundant reactive groups in PDA, the PAM/BA-Ag@PDA hydrogel exhibits inherent tissue adhesiveness and antioxidant, along with a synergistic antibacterial effect by PDA and Ag. Toward practical applications, the PAM/BA-Ag@PDA hydrogel can conformally adhere to skin and monitor subtle activities and large-scale movements with excellent reliability, demonstrating its promising applications as wearable sensors for healthcare.

研究领域: 材料科学 · 生物医学工程 · 纳米技术 · 传感器与执行器
✓ 已验证 DOI 高影响因子
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APPLIED ORGANOMETALLIC CHEMISTRY · 2020 ·Vol. 34 ·期 10 ·e5814 · IF 3.14

Hollow N-ZIFs@NiCo-LDH as highly efficient catalysts for 4-nitrophenol and dyes

Yongcen Lin,Xue Dong,Lang Zhao

N-ZIF-(1:0)@NiCo-LDH, N-ZIF-(1:3.5)@NiCo-LDH and N-ZIF-(0:1)@NiCo-LDH were prepared by mixing solvents in various volume ratios ( V methanol : V water = 1:0, 1:3.5 and 0:1) when synthesizing precursors. These composite materials were characterized using scanning and transmission electron microscopies, X-ray diffraction, X-ray photoelectron spectroscopy and nitrogen adsorption–desorption measurements, and investigated as catalysts for reduction of 4-nitrophenol, methyl orange and methylene blue. The NaBH 4 concentration as an important factor that may affect catalytic activity for reduction of 4-nitrophenol was examined. Under optimal experimental conditions, the excellent catalytic activity of the N-ZIF-(0:1)@NiCo-LDH composite, compared to that of N-ZIF-(1:0)@NiCo-LDH and N-ZIF-(1:3.5)@NiCo-LDH composites, could be attributed to the presence of graphitic nitrogen. In addition, compared with previously reported catalysts, all catalysts prepared show excellent catalytic activity owing to the unique structure exposing more active sites.

研究领域: 材料科学 · 环境化学 · 催化化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2017 ·Vol. 28 ·期 16 ·11563-11568 · IF 2.019

Borosiloxane boron diffusion for p-emitter formation on n-type silicon wafers

Sun Xinjie,Tong Hua,Yuan Xiao,Liu Cui,Yuan Shuanglong,Chen Guorong,Yang Yunxia

Thermal boron diffusion, which forms highly doped and shallow p-emitters on phosphor-doped silicon wafers, is one of the primary processes in commercial-scale production of n-type cells. Here, we report on the use of nontoxic and nonvolatile borosiloxane sols as the spin-on boron source. In comparison to the tribromide (BBr 3 ) boron diffusion that is applied in the production of most commercial n-type cells, borosiloxane boron diffusion may have potential advantages in terms of cost, safety, operability, etc. The borosiloxane sols studied here were formed from a cross-linking reaction between boron acid and a mixture of two types of silicon alkoxides, methyltriethoxysilane (MTEOS) and dimethyldiethoxysilane (DMDEOS). The MTEOS/DMDEOS ratio was found to be the key factor determining the synthetic period, net structure, thermal transformation property, and coating behavior of the borosiloxane sols. In combination with the spin-coating method, the performance of borosiloxane boron diffusion into phosphor-doped silicon wafers (1–3 Ω·cm) was systematically investigated by varying the borosiloxane composition (boron/silicon or MTEOS/DMDEOS ratio) and the diffusion process parameters (temperature, ambience, and period of individual sub-steps), and by relating them to the resulting sheet resistance and boron doping profile. The results show that under the diffusion conditions in conventional cell production lines, the formed p-emitters can have variable sheet resistance in the range of 35–582 Ω/□ and boron doping depth of 100–300 nm.

研究领域: 材料科学 · 半导体物理 · 光伏技术 · 表面工程 · 纳米材料 · 化学气相沉积 · 微电子学
✓ 已验证 DOI 高影响因子
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 27 ·13010-13020 · IF 3.925

Facile preparation of BiOI/T-ZnOw p–n heterojunction photocatalysts with enhanced removal efficiency for rhodamine B and oxytetracycline

Jianke Tang,Yanfeng Xue,Chunlei Ma,Shengjian Zhang,Qiaoling Li

The construction of p–n heterojunctions instead of p-type or n-type semiconductors can improve the separation efficiency of photoinduced electrons and holes. In this work, BiOI/tetrapod-like ZnO whisker (T-ZnOw) p–n heterojunction photocatalysts with different Bi/Zn molar ratios were prepared by the in situ precipitation of BiOI on a T-ZnOw substrate. The BiOI/T-ZnOw photocatalysts efficiently degraded rhodamine B (RhB) and oxytetracycline (OTC) under visible light irradiation. The photocatalyst with a Bi/Zn molar ratio of 1 : 10 (BZ-10) exhibited the highest photocatalytic activity, with 97.1% and 88.0% removal of RhB and OTC, respectively. After degradation cycling experiments, the OTC removal efficiency was still 80.7%. The photocatalytic activity of the BZ-10 composite was improved compared to those of pure T-ZnOw and BiOI. This was attributed to the large specific surface area and the efficient separation of charge carriers caused by the formation of p–n heterojunctions between BiOI and T-ZnOw. The photodegradation mechanism was put forward based on radical trapping experiments and electron spin resonance (ESR) results. The synthesized BiOI/T-ZnOw heterojunction composite could be a promising photocatalyst in environmental photocatalysis.

研究领域: 环境科学 · 材料科学
✓ 已验证 DOI 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Construction of Ni-based N-doped mesoporous carbon sphere for efficiently catalytic dichromate reduction with HCOOH at room temperature

Zhimin Lv,Shuya Liu,Yuxin Liu,Peisheng Liu,Ming Fang,Xiaoli Tan,Wei Xu,Mingguang Kong,Xiangke Wang

The pollution of poisonous Cr(VI) poses a severe threat to our health, and the reduction of Cr(VI) to Cr(III) has become a high-efficiency way for wastewater remediation. Herein, the catalyst with metallic Ni confined in an N-doped mesoporous carbon sphere was prepared by the easy pyrolysis method of carbon sphere with Ni salts and showed remarkable activity, selectivity, and stability for reducing Cr(VI) with HCOOH. Notably, the Ni-N-C600 can rapid and 100 % reduction of the high concentrations of Cr(VI) (100 mg/L, 100 ml) using HCOOH within 7 min at room temperature over the reported Ni-based catalysts. Even in the presence of coexisting ions (0.1 M of Na + , K + , Ca 2+ , Zn 2+ , NO 3 − , Cl − , CO 3 2− , and SO 4 2− ), its catalytic efficiency is not affected at all. The catalytic activity of the Ni-N-C600 declined little even after five cycles because the confinement effect of the mesoporous carbon sphere physical barrier prevented the leaching and aggregation of Ni NPs. The magnetism of metallic Ni greatly facilitates the separation of the catalyst. The reduction mechanism is mainly achieved by active hydrogen produced through the dehydrogenation of HCOOH. In addition, the electronic donation of C-containing functional groups also caused a partial reduction of Cr(VI). This work provides a rational design and development of high-efficiency non-noble metal catalysts to reduce Cr(VI).

研究领域: 环境科学 · 材料科学
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING SCIENCE · 2024 · IF 4.1

Role of hydrogen spillover on the hydrogenation of N-ethylcarbazole over in-situ Encapsulation of Ru within zeolite for hydrogen storage

Yibo Qin,Longfei Chen,Lixia Ge,Yanfeng Zhu,Wanting Li,Xinxin Cao,Tianchang Wang,Jiong Li,Wei Han,Xinqing Chen

Hydrogen spillover plays a crucial role in heterogeneous catalysis, significantly enhancing the activity of catalysts. However, the promotion mechanism of hydrogen spillover on non-reducible oxide supports (such as zeolite) is rarely reported. Herein, we prepared Ru@Beta sample by in-situ approach, effectively encapsulating Ru species into Beta zeolite. Additionally, three samples (Ru/SiO 2 , Ru@Naβ, and Ru@Hβ) with different hydrogen spillover effect were prepared. The optimal concentration of Ru was 0.5 wt%, and the Ru@Hβ sample with the strongest hydrogen spillover has 100 % conversion rate of N-ethylcarbazole (NEC) and 98 % selectivity towards to 12H-NEC. In contrast, the Ru/SiO 2 with weak hydrogen spillover has only 89.5 % conversion rate and 28.9 % selectivity of 12H-NEC. Notably, the Ru@Hβ can still completely convert NEC even after 7 cycles, thereby exhibiting its remarkable activity and stability. Various characterizations (HAADF-STEM, XPS, EXAFS, in-situ DRIFT, and H 2 -TPD) indicate the superior catalytic performance of Ru@Hβ with strong hydrogen spillover effect, originating from the presence of more hydroxyl (–OH) and Brønsted acid on the surface, while Lewis acid act as hydrogen acceptors and NEC hydrogenation sites. This work not only expands our understanding of the hydrogen spillover, but also paves the way onto the potential applications in heterogeneous catalysis for efficient hydrogenation.

研究领域: 催化化学 · 材料科学 · 能源存储
✓ 已验证 DOI 高影响因子
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2023 ·Vol. 170 ·期 7 ·077509 · IF 3.9

MOF-derived Cu/N–C Composite Based Electrochemical Sensor for Simultaneous Detection of Catechol and Hydroquinone

Qi Wang,Wenjing Liu,Jinjin Zhang,Jianying Qu

In this work, Cu/N-C derived from MOF composites were synthesized and characterized by SEM, XRD, FTIR, XPS and EIS, which was modified on the glassy carbon electrode (GCE) to construct a novel electrochemical sensor (Cu/N-C/GCE). Due to the good electrical conductivity and abundant catalytic active sites of Cu/N-C, Cu/N-C/GCE exhibited excellent electrocatalytic performance for catechol (CC) and hydroquinone (HQ) with the oxidation peak potential difference of 112 mV. The proposed sensor could realize the simultaneous detection of CC and HQ successfully. Under optimal conditions, the redox peak currents of both CC and HQ have good linear relationship with their concentrations in the ranges of 0.50–100.00 μM and 0.50–150.00 μM with the detection limits for CC and HQ of 0.12 μM and 0.09 μM, respectively. At the same time, the sensor exhibits good stability, reproducibility and selectivity in the analysis of practical samples.

研究领域: 分析化学 · 材料科学 · 环境科学
✓ 已验证 DOI 高影响因子
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MOLECULES · 2023 ·Vol. 29 ·期 1 ·83 · IF 4.6

Design, Synthesis, and Antifungal Activity of N-(alkoxy)-Diphenyl Ether Carboxamide Derivates as Novel Succinate Dehydrogenase Inhibitors

Bo He,Yanhao Hu,Wang Chen,Xu He,Enpei Zhang,Mengxu Hu,Pu Zhang,Wei Yan,Yonghao Ye

Succinate dehydrogenase (SDH, EC 1.3.5.1) is one of the most promising targets for fungicide development and has attracted great attention worldwide. However, existing commercial fungicides targeting SDH have led to the increasingly prominent problem of pathogen resistance, so it is necessary to develop new fungicides. Herein, we used a structure-based molecular design strategy to design and synthesize a series of novel SDHI fungicides containing anN-(alkoxy)diphenyl ether carboxamide skeleton. The mycelial growth inhibition experiment showed that compoundM15exhibited a very good control effect against four plant pathogens, with inhibition rates of more than 60% at a dose of 50 μg/mL. A structure–activity relationship study found that N-O-benzyl-substituted derivatives showed better antifungal activity than others, especially the introduction of a halogen on the benzyl. Furthermore, the molecular docking results suggested that π–π interactions with Trp35 and hydrogen bonds with Tyr33 and Trp173 were crucial interaction sites when inhibitors bound to SDH. Morphological observation of mycelium revealed thatM15could inhibit the growth of mycelia. Moreover, in vivo and in vitro tests showed thatM15not only inhibited the enzyme activity of SDH but also effectively protected rice from damage due toR. solaniinfection, with a result close to that of the control at a concentration of 200 μg/mL. Thus, theN-(alkoxy)diphenyl ether carboxamide skeleton is a new starting point for the discovery of new SDH inhibitors and is worthy of further investigation.Keywords:succinate dehydrogenase (SDH);antifungal activity;fungicide;N-(alkoxy)diphenyl ether carboxamide

研究领域: 药理学 · 植物病理学 · 化学生物学
✓ 已验证 DOI PubMed 高影响因子
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Molecular Catalysis · 2018 · IF 0

N-doped hierarchical porous carbon anchored tiny Pd NPs: A mild and efficient quinolines selective hydrogenation catalyst

Fengwei Zhang,Chunlan Ma,Shuai Chen,Jianfei Zhang,Zhihong Li,Xian-Ming Zhang

Chemoselective hydrogenation of quinolines is often subjected to the problems of leaching and poisoning of catalytic active site as well as harsh reaction conditions. Developing a novel and high-performance heterogeneous catalyst is of paramount importance yet a huge challenge. Herein, we report a facile and efficient strategy for preparing the large surface area and highly N-doped hierarchical porous carbon anchored tiny Pd NPs catalyst, in which the low-cost chitosan, nitrogen-rich ionic liquids are served as composite precursors and KZ molten salt as friendly pore-forming agent. And a series of Pd@CIL-T (C refers to chitosan, IL refers to ionic liquid, T = 600–900 °C) catalysts are successfully fabricated via pyrolyzing aforesaid composites at different temperatures followed by anchoring the highly dispersed and small-sized Pd NPs on their surface. Among all the prepared catalysts, Pd@CIL-900 exhibits the optimal catalytic performance towards the selective hydrogenation of quinoline under extremely mild conditions (0.6 mol% Pd, 0.1 MPa H 2 and 50 °C). The kinetic experiments further reveal that such hydrogenation is subject to a pseudo-first order reaction and the apparent activation energy is as low as 41.1 kJ/mol, demonstrating excellent hydrogenation reaction rate. Moreover, the catalytic activity and selectivity are well maintained even after being reused for fifth reaction cycles.

研究领域: 化学 · 催化材料 · 纳米技术
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Selective adsorption and high recovery of La3+ using graphene oxide/poly (N-isopropyl acrylamide-maleic acid) cryogel

Xinwei Yang,Dereje Kebebew Debeli,Guorong Shan,Pengju Pan

The increasing use of rare earth elements (REEs) in a wide range of high-tech applications, leading to global ever-increasing demands, has stimulated the development of new technologies for REEs separation and recovery. Herein, an efficient porous graphene oxide/poly ( N -isopropyl acrylamide-maleic acid) [GO/P(NIPAM-MA)] cryogel was synthesized by cryopolymerization and was employed as the REEs recovery adsorbent. The cryogel exhibits stable, microporous interpenetrating structure and thermosensitive characteristics. The adsorption follows the pseudo-second-kinetic model indicating that the adsorption process was controlled by the adsorption sites with the equilibrium adsorption capacity of La 3+ was 33.1 mg/g. The Langmuir isotherm model fits the data better, revealing the homogenous adsorption for REEs on the surface of the adsorbent. Besides, the adsorbent displayed preferential adsorption of La 3+ compared to Cu 2+ , Co 2+ , Ni 2+ , Nd 3+ , Yb 3+ in a binary solution suggested the high level of La 3+ separation efficiency that exceeded 95%. In general, the eco-friendly, sustainability and higher efficiency characteristics of GO/P(NIPAM-MA) cryogel provide a promising route for recycling rare earth elements from wastewater.

研究领域: 材料科学 · 环境科学
✓ 已验证 DOI 高影响因子
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