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CHINESE JOURNAL OF CATALYSIS · 2024 · IF 15.7

Identification of origin of insulating polymer maneuvered photoredox catalysis

Qiao-Ling Mo,Rui Xiong,Jun-Hao Dong,Bai-Sheng Sa,Jing-Ying Zheng,Qing Chen,Yue Wu,Fang-Xing Xiao

ABSTRACT Solid non-conjugated polymers have long been regarded as insulators due to deficiency of delocalized π electrons along the molecular chain framework. Up to date, origin of insulating polymer regulated charge transfer has not yet been uncovered. In this work, we unleash the root origin of charge transport capability of insulating polymer in photocatalysis. We ascertain that insulating polymer plays crucial roles in fine tuning of electronic structure of transition metal chalcogenides (TMCs), which mainly include altering surface electron density of TMCs for accelerating charge transport kinetics, triggering the generation of defect over TMCs for prolonging carrier lifetime, and acting as hole-trapping mediator for retarding charge recombination. These synergistic roles contribute to the charge transfer of insulating polymer. Our work opens a new vista of utilizing solid insulating polymers for maneuvering charge transfer toward solar energy conversion.

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CHINESE JOURNAL OF CATALYSIS · 2024 · IF 15.7

Mo-promoted Pd/NaY catalyst for indirect oxidative carbonylation of methanol to dimethyl carbonate

Ke Huang,Shicheng Yuan,Rongyan Mei,Ge Yang,Peng Bai,Hailing Guo,Chunzheng Wang,Svetlana Mintova

A chlorine-free catalyst consisting of zeolite Y modified with Pd (Pd/NaY) catalyst has been prepared and used in the indirect oxidative carbonylation of methanol to dimethyl carbonate (DMC). The activity and stability of the catalyst were further improved by introducing molybdenum into Pd/NaY using a top-down approach (Pd-Mo/NaY catalyst). The Pd-Mo/NaY catalyst exhibited higher stability compared to the Pd/NaY. A high CO conversion of 97% and DMC selectivity of 80% during a 30-hour catalytic test for the Pd-Mo/NaY were obtained. Furthermore, the incorporation of Mo was found to partially heal the silanols and hinder the aggregation of Pd in the Pd-Mo/NaY catalyst. The interactions between Mo and Pd increased the amount of active Pd 2+ species and enhanced the adsorption of CO reactant on the Pd-Mo/NaY catalyst. The key reaction intermediate of COOCH 3 * was captured by in situ diffuse reflectance infrared Fourier transform spectroscopy . The stabilization of active Pd 2+ species contributed to the enhanced catalytic activity of the Pd-Mo/NaY catalyst in the indirect oxidative carbonylation of methanol to DMC reaction.

CAS / MDL: 1302-42-7
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CHINESE JOURNAL OF CATALYSIS · 2018 · IF 3.525

Composition-controlled synthesis of platinum and palladium nanoalloys as highly active electrocatalysts for methanol oxidation

Haiqiang Zhao,Weihong Qi,Xinfeng Zhou,Haofei Wu,Yejun Li

Platinum and palladium (PtPd) alloy nanoparticles (NPs) are excellent catalysts for direct methanol fuel cells. In this study, we developed PtPd alloy NPs through the co-reduction of K 2 PtCl 4 and Na 2 PdCl 4 in a polyol synthesis environment. During the reaction, the feed molar ratio of the two precursors was carried over to the final products, which have a narrow size distribution with a mean size of approximately 4 nm. The catalytic activity for methanol oxidation reactions possible depends closely on the composition of as-prepared PtPd alloy NPs, and the NPs with a Pt atomic percentage of approximately 75% result in higher activity and stability with a mass specific activity that is 7 times greater than that of commercial Pt/C catalysts. The results indicate that through composition control, PtPd alloy NPs can improve the effectiveness of catalytic performance.

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CHINESE JOURNAL OF CATALYSIS · 2018 · IF 3.525

Enhanced Fenton, photo-Fenton and peroxidase-like activity and stability over Fe3O4/g-C3N4 nanocomposites

Shafaq Sahar,Akif Zeb,Yanan Liu,Naseeb Ullah,Anwu Xu

We prepared the Fe 3 O 4 /g-C 3 N 4 nanoparticles (NPs) through a simple electrostatic self-assembly method with a 3:97 weight ratio to investigate their Fenton , photo-Fenton and oxidative functionalities besides photocatalytic functionality. We observed an improvement of the Fenton and photo-Fenton activities of the Fe 3 O 4 /g-C 3 N 4 nanocomposites . This improvement was attributed to efficient charge transfer between Fe 3 O 4 and g-C 3 N 4 at the heterojunctions, inhibition of electron-hole recombination, a high surface area, and stabilization of Fe 3 O 4 against leaching by the hydrophobic g-C 3 N 4 . The obtained NPs showed a higher degradation potential for rhodamine B (RhB) dye than those of Fe 3 O 4 and g-C 3 N 4 . As compared to photocatalysis , the efficiency of RhB degradation in the Fenton and photo-Fenton reactions was increased by 20% and 90%, respectively. Additionally, the horseradish peroxidase (HRP) activity of the prepared nanomaterials was studied with 3,3,5,5-tetramethylbenzidinedihydrochloride (TMB) as a substrate. Dopamine oxidation was also examined. Results indicate that Fe 3 O 4 /g–C 3 N 4 nanocomposites offers more efficient degradation of RhB dye in a photo-Fenton system compared with regular photocatalytic degradation, which requires a long time. Our study also confirmed that Fe 3 O 4 /g-C 3 N 4 nanocomposites can be used as a potential material for mimicking HRP owing to its high affinity for TMB. These findings suggest good potential for applications in biosensing and as a catalyst in oxidation reactions.

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CHINESE JOURNAL OF CATALYSIS · 2024 · IF 15.7

Efficient electrocatalytic urea synthesis from CO2 and nitrate over the scale-up produced FeNi alloy-decorated nanoporous carbon

Zuo-Shu Sun,Xue-Yan Xiang,Qiu-Ping Zhao,Zhao Tang,Shi-Yi Jiang,Tong-Bu Lu,Zhi-Ming Zhang,Baifan Wang,Hua-Qing Yin

Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis, but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging. Herein, we developed a simple method for the preparation of a series of FeNi-alloy-based catalysts, named FeNi@ n C- T ( n represents the content of nanoporous carbon as 1, 3, 5, 7 or 9 g and T = 900, 950, 1000 or 1100 °C), for highly performed urea synthesis via NO 3 − and CO 2 co-reduction. The FeNi@7C-1000 achieved a high urea yield of 1041.33 mmol h −1 g FeNi −1 with a Faradaic efficiency of 15.56% at –1.2 V vs . RHE. Moreover, the scale-up synthesized FeNi@7C-950-S (over 140 g per batch) was achieved with its high catalytic performance and high stability maintained. Mechanism investigation illuminated that the Ni and Fe sites catalyze and stabilize the key *CO and *N intermediates and minimize the C–N coupling reaction barriers for highly efficient urea synthesis.

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CHINESE JOURNAL OF CATALYSIS · 2025 · IF 17.7

Dimethoxymethane carbonylation and disproportionation over extra-large pore zeolite ZEO-1: Reaction network and mechanism

Shaolei Gao,Peng Lu,Liang Qi,Yingli Wang,Hua Li,Mao Ye,Valentin Valtchev,Alexis T. Bell,Zhongmin Liu

Methyl methoxyacetate (MMAc) and methyl formate (MF) can be produced directly by heterogeneous zeolite-catalyzed carbonylation and disproportionation of dimethoxymethane (DMM), with near 100% selectivity for each process. Despite continuous research efforts, the insight into the reaction mechanism and kinetics theory are still in their nascent stage. In this study, ZEO-1 material, a zeolite with up to now the largest cages comprising 16×16-MRs, 16×12-MRs, and 12×12-MRs, was explored for DMM carbonylation and disproportionation reactions. The rate of MMAc formation based on accessible Brönsted acid sites is 2.5 times higher for ZEO-1 (Si/Al = 21) relative to the previously investigated FAU (Si/Al = 15), indicating the positive effect of spatial separation of active sites in ZEO-1 on catalytic activity. A higher MF formation rate is also observed over ZEO-1 with lower activation energy (79.94 vs. 95.19 kJ/mol) compared with FAU (Si/Al = 30). Two types of active sites are proposed within ZEO-1 zeolite: Site 1 located in large cages formed by 16×16-MRs and 16×12-MRs, which is active predominantly for MMAc formation, and Site 2 located in smaller cages for methyl formate/dimethyl ether formation. Kinetics investigation of DMM carbonylation over ZEO-1 exhibit a first-order dependence on CO partial pressure and a slightly inverse-order dependence on DMM partial pressure. The DMM disproportionation is nearly first-order dependence on DMM partial pressure, while it reveals a strongly inverse dependence with increasing CO partial pressure. Furthermore, ZEO-1 exhibits good catalytic stability, and almost no deactivation is observed during the more than 70 h test with high carbonylation selectivity of above 89%, due to the well-enhanced diffusion property demonstrated by intelligent-gravimetric analysis.

CAS / MDL: 109-87-5
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European Physical Journal Plus · 2024 ·Vol. 139 ·期 7 ·1-9 · IF 2.8

Electrospun fluorinated poly(aryl ether) fiber membrane: preparation and high triboelectric output performance

Wang Zhaoyang,Yang Huawei,Qi Yonggang,Wang Lifei,Zou Jiawei

Abstract As unique class of specialty engineering plastics, the development and applications for poly(aryl ether)s is of utmost significance in energy field due to their outstanding heat resistance and mechanical properties in highly challenging environments. Thus, In this study, fluorinated poly(aryl ether) fiber membrane (FPAE-FM) is successfully prepared by electrospinning technology. Furthermore, FPAE-FM is paired with copper to construct a vertical contact-separated triboelectric nanogenerator (TENG). The open-circuit voltage is 75 V and the short-circuit current is 3 μA. The construction of fiber increases the surface roughness of FPAE-FM, which facilitates the generation of triboelectric charges and improve the surface charge density. Furthermore, SiO 2 is introduced into FPAE-FM, which not only improves the surface roughness of the fibers to a certain extent, but also builds charge trap at the interface between SiO 2 and FPAE for trapping triboelectric charges, reducing the charge dissipation and increasing the volume charge density. The collective augmentation of surface charge density and volume charge density synergistically enhances the triboelectric output performance, resulting in a remarkable surge in both the open-circuit voltage and short-circuit current of TENG, reaching 147 V and 11 μA, respectively. Overall, this study provides new materials and theoretical support for exploiting TENG with high-performance. Graphical abstract

CAS / MDL: 434-90-2 584-08-7
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CHINESE JOURNAL OF CATALYSIS · 2024 · IF 15.7

Engineering the coordination structure of Cu for enhanced photocatalytic production of C1 chemicals from glucose

Lulu Sun,Shiyang Liu,Taifeng Liu,Dongqiang Lei,Nengchao Luo,Feng Wang

ABSTRACT Photocatalytic decomposition of sugars is a promising way of providing H 2 , CO, and HCOOH as sustainable energy vectors. However, the production of C 1 chemicals requires the cleavage of robust C−C bonds in sugars with concurrent production of H 2 , which remains challenging. Here, the photocatalytic activity for glucose decomposition to HCOOH, CO (C 1 chemicals), and H 2 on Cu/TiO 2 was enhanced by nitrogen doping. Owing to nitrogen doping, atomically dispersed and stable Cu sites resistant to light irradiation are formed on Cu/TiO 2 . The electronic interaction between Cu and nitrogen ions originates valence band structure and defect levels composed of N 2 p orbit, distinct from undoped Cu/TiO 2 . Therefore, the lifetime of charge carriers is prolonged, resulting in the production of C 1 chemicals and H 2 with productivities 1.7 and 2.1 folds that of Cu/TiO 2 . This work provides a strategy to design coordinatively stable Cu ions for photocatalytic biomass conversion.

CAS / MDL: 71-23-8
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CHINESE JOURNAL OF CATALYSIS · 2025 · IF 17.7

A visible-light-driven CoS2/CuS@CNT-C3N4 photocatalyst for high-performance rechargeable zinc-air batteries beyond 500 mW cm–2

Yang Zhang,Nengneng Xu,Bingbing Gong,Xiaoxiao Ye,Yi Yang,Zhaodi Wang,Biyan Zhuang,Min Wang,Woochul Yang,Guicheng Liu,Joong Kee Lee,Jinli Qiao

Storing solar energy in battery systems is crucial to achieving a green and sustainable society. However, the efficient development of photo-enhanced zinc-air batteries (ZABs) is limited by the rapid recombination of photogenerated carriers on the photocathode. In this work, the visible-light-driven CoS 2 /CuS@CNT-C 3 N 4 photocatalyst with unique petal-like layer structure was designed and developed, which can be used as air electrode for visible-light-driven ZABs. The superior performance of ZABs assembled by CoS 2 /CuS@CNT-C 3 N 4 was mainly attributed to the successful construction of Schottky heterojunction between g-C 3 N 4 and carbon nanotubes (CNTs), which accelerates the transfer of electrons from g-C 3 N 4 to CoS 2 /CuS cocatalysts, improves the carrier separation ability, and extends the carrier lifetime. Thereinto, the visible-driven ZABs assembled by CoS 2 /CuS@CNT-C 3 N 4 photocatalyst has a power density of 588.90 mW cm –2 and a charge-discharge cycle of 643 h under visible light irradiation, which is the highest performance ever reported for photo-enhanced ZABs. More importantly, the charge-discharge voltage drop of ZABs was only 0.54 V under visible light irradiation, which is significantly lower than the voltage drop (0.94 V) in the dark. This study provides a new idea for designing efficient and stable visible-light-driven ZABs cathode catalysts.

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CHINESE JOURNAL OF CATALYSIS · 2024 · IF 15.7

Adjusting Al location in the framework of ITH zeolites for catalytic conversion of methanol to olefins

Kai Fan,Qinming Wu,Shuo Liu,Haiyu Kong,Sen Wang,Eduard Kunkes,Trees De Baerdemaeker,Andrei-Nicolae Parvulescu,Nils Bottke,Toshiyuki Yokoi,Dirk E. De Vos,Xiangju Meng,Weiping Zhang,Feng-Shou Xiao

Adjusting location and distribution of Al sites in the zeolite framework is critical for catalysis, and typical strategies include using zeolites as starting Al source. However, this approach is still challenging for aluminosilicate ITH zeolite. Herein, the distribution of Al species in the framework of ITH was efficiently regulated by implementing LTA zeolite as the aluminum source added in the starting gels (LTA-ITH). The obtained LTA-ITH zeolites have similar nanosheet morphology, textual parameters, and acidic properties to those of conventional ITH synthesized from boehmite (C-ITH), while the results of 27 Al MAS NMR spectra and 1-hexene cracking indicate that they have a different Al distribution. The use of LTA zeolite in starting gel is favorable for the formation of more Al species in sinusoidal and straight channels, compared with the C-ITH. Catalytic tests in the conversion of methanol to light olefin showed that LTA-ITH exhibited enhanced catalyst lifetime and propene selectivity compared with the C-ITH, which is reasonably attributed to the different locations of Al species in their respective ITH frameworks.

CAS / MDL: 110-52-1 78-10-4
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Chinese Journal of Natural Medicines · 2024 · IF 4

Repurposing diacerein to suppress colorectal cancer growth by inhibiting the DCLK1/STAT3 signaling pathway

Qiaobei YE,Yu ZHU,Meng SHI,Linxi LV,Yuyan GONG,Luyao ZHANG,Lehe YANG,Haiyang ZHAO,Chengguang ZHAO,Huanhai XU

ABSTRACT Double cortin-like kinase 1 (DCLK1) exhibits high expression levels across various cancers, notably in human colorectal cancer (CRC). Diacerein, a clinically approved interleukin (IL)-1β inhibitor for osteoarthritis treatment, was evaluated for its impact on CRC proliferation and migration, alongside its underlying mechanisms, through both in vitro and in vivo analyses. The study employed MTT assay, colony formation, wound healing, transwell assays, flow cytometry, and Hoechst 33342 staining to assess cell proliferation, migration, and apoptosis. Additionally, proteome microarray assay and western blotting analyses were conducted to elucidate diacerein’s specific mechanism of action. Our findings indicate that diacerein significantly inhibits DCLK1-dependent CRC growth in vitro and in vivo . Through high-throughput proteomics microarray and molecular docking studies, we identified that diacerein directly interacts with DCLK1. Mechanistically, the suppression of p-STAT3 expression following DCLK1 inhibition by diacerein or specific DCLK1 siRNA was observed. Furthermore, diacerein effectively disrupted the DCLK1/STAT3 signaling pathway and its downstream targets, including MCL-1, VEGF, and survivin, thereby inhibiting CRC progression in a mouse model, thereby inhibiting CRC progression in a mouse model.

CAS / MDL: 108-18-9
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CHINESE JOURNAL OF CATALYSIS · 2025 · IF 17.7

Work function-induced spontaneous built-in electric field in Ir/MoSe2 for efficient PEM water electrolysis

Bingjie Zhang,Chunyan Wang,Fulin Yang,Shuli Wang,Ligang Feng

Bifunctional Ir catalysts for proton exchange membrane (PEM) water electrolysis offer transformative potential by streamlining electrolyzer while achieving efficient performance remains challenging due to the distinct conditions required for oxygen and hydrogen evolution reaction (OER and HER). Herein, we propose a theory-directed design of Ir-based bifunctional catalysts, Ir nanoparticles supported on mesoporous carbon spheres embedded with MoSe 2 (Ir/MoSe 2 @MCS), leveraging a work function (WF)-induced spontaneous built-in electric field to enhance catalytic performance. They demonstrate exceptional kinetics for both OER and HER, and potential application in the practical PEM electrolyzer, showcasing the effectiveness of this innovative approach. Low overpotentials of 252 mV for OER and 28 mV for HER to drive 10 mA cm –2 were observed, and the PEM electrolyzer showed the current density of 2 A cm –2 at 1.87 V and maintained stable activity at 1.65 V for over 30 h to deliver 1 A cm –2 . Density functional theory calculations reveal that the WF difference at Ir/MoSe 2 interface induces a spontaneous built-in electric field with asymmetric charge distributions, that modulate the electronic environment and d -band center of Ir promoting bifunctional active phase formation. This significantly lowers reaction barriers for water splitting by balancing intermediate adsorption, endowing the bifunctional activity.

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