GREEN CHEMISTRY
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2026
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IF 9.2
Yi Xu,Fanshu Yuan,Xiaotian Xie,Jinhui Tong,Cheng Min,Qian Zhang,Jie Tang,Jie Liu,Tingting Lv,Qianli Zhang
Activating lattice oxygen in oxygen evolution reactions (OER) serves as an effective strategy to overcome the inherent limitations of the traditional adsorbate evolution mechanism (AEM). Molybdenum dioxide (MoO2), which has attracted attention due to its high electrical conductivity and other metallic properties, exhibits excessive adsorption of oxygen-containing intermediates at its elevated molybdenum d-band center. This leads to the formation of stable Mo–O bonds, thereby hindering the lattice oxygen mechanism (LOM). This study demonstrates that phosphorus doping serves as a more direct strategy for intrinsic electronic structure modulation. DFT calculations predict that phosphorus doping effectively lowers the d-band center of molybdenum and softens Mo–O bonds, thereby enabling lattice oxygen participation in the reaction mechanism. Consistent with the computational results, experimental kinetic studies (e.g., pH-dependent experiments) and chemical probe tests confirm that P-MoO2 follows the LOM pathway. The prepared P-MoO2 catalyst exhibits an overpotential of only 247 mV at 10 mA cm−2 current density while maintaining stability for up to 100 hours. Furthermore, through various characterization techniques (TEM, XPS, in situ Raman spectroscopy), it was observed that the catalyst underwent significant potential-induced surface reconstruction during the reaction process, forming an amorphous MoO(OH)x layer rich in Mo5+. This reconstructed layer is considered the true active phase, where Mo5+ has been confirmed as the dominant valence state in the OER process.
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Journal of Inorganic and Organometallic Polymers and Materials
·
2013
·Vol. 23
·期 6
·1492-1500
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IF 1.174
Zhang Nan,Fan Yu-Hua,Bi Cai-Feng,Zhang Xia,Zhang Peng-Fei,Zhang Zhong-Yu,Li Xin
Three novel transition metal coordination polymers, [Ni(C 18 H 16 N 3 O 2 ) 2 ·2CH 3 OH]
n
( 1 ), [Zn(C 18 H 16 N 3 O 2 ) 2 ·4CH 3 OH]
n
( 2 ) and [Cd(C 18 H 16 N 3 O 2 ) 2 ·2CH 3 OH]
n
( 3 ) (C 18 H 16 N 3 O 2 =2-acetylpyridine- d -tryptophan) were synthesized and characterized by elemental analysis, IR, UV, 1 H NMR and X-ray diffraction single crystal analysis. The analyses of the structures indicate that all three materials crystallize in the tetragonal crystal system, space group P 4 1 2 1 2. They have similar structures; i.e., the Schiff base coordinates in its deprotonated form and behaves as a hexadentate (4N+2O) coordinated ligand to form a distorted octahedron geometry. On the other hand, as a result of the alternate arrangement of chains through N–H···O intermolecular hydrogen bonds interactions, 2-D layers are formed for the three complexes. Furthermore, the luminescent properties and thermal stabilities of the three complexes were investigated.
研究领域:
无机化学
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配位化学
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材料化学
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晶体工程
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光物理化学
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Science China-Chemistry
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2026
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IF 9.8
Wang Nan,An Tinghui,Li Jiaqi,Wang Yuhao,Xiang Dong,Cai Kedi
Cu-based electrocatalysts are promising for the electrocatalytic CO 2 reduction reaction (eCO 2 RR) to realize valuable chemicals production. Here, a Mg-doped Cu based electrocatalysts via transient CO 2 pulsed laser (L 4 -Mg/Cu x O) was synthesized for highly selective eCO 2 RR to ethanol (C 2 H 5 OH). The synergistic effect of Mg-doping and transient CO 2 pulsed laser irradiation enables excellent eCO 2 RR performance, realizing Faradaic efficiencies (FE) of 52.2% and 74.1% for C 2 H 5 OH and C 2 products under a high current density of 298.9 mA cm −2 , respectively. Operando Raman spectroscopy and DFT simulations results confirm that Mg-doping strategy suppresses the hydrogen evolution reaction (HER), enhances CO adsorption, elevates local pH and accelerates H 2 O dissociation, which could be beneficial for promoting OC–CO coupling and proton supply in eCO 2 RR. Furthermore, Mg incorporation induces electron delocalization in which electron accumulation on the C atom of *CHCOH intermediate and its enhanced p-d orbital coupling with Cu interface, which stabilizes the C–O bond from breakage and selectively favours the C 2 H 5 OH pathway, thus decoupling the selectivity between C 2 H 5 OH and ethylene. When employed in Li-CO 2 batteries, L 4 -Mg/Cu x O delivers 20480 mAh g −1 discharge capacity and cycling stability over 187 cycles. This work presents a universal strategy for regulating eCO 2 RR selectivity through precise laser energy delivery, demonstrating significant potential for renewable energy conversion and storage.
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ACS Catalysis
·
2026
·
IF 13.6
Shunwu Wang,Zhenbo Guo,Bing Tang,Jinglin Du,Qianling Zou,Ligang Wang,Xiaohui Li,Xiaodong Zhou,Lang Liu,Yadong Li
Developing chemoselective hydrogenation of alkynes into alkenes is one of the major strategies of the fine chemical industry; however, it presents significant challenges in achieving the semi-hydrogenation of carbon−carbon triple bond (C=C) to carbon−carbon double bond (C=C) without further hydrogenation. Herein, it is proposed that d−p orbital hybridization between the Pd single-atom-cluster sites and the bismuth species can serve as a descriptor for revealing the catalytic activity. Guided by DFT simulation, the well-dispersed Pd clusters and single-atom Pd−O4 sites on Bi-doped hydroxyapatite (PdSA+C/HAP-Bi) are fabricated for semi-hydrogenation of phenylacetylene, realizing the trade-off between activity and selectivity with a robust turnover frequency of 10,140 h−1, surpassing those of the commercial Pd/C catalyst and most of the reported catalysts. It also displays good stability for enduring six cycles with minimal declines in conversion and selectivity. Notably, this catalyst offers a general platform, showcasing broad substrate compatibility across at least 30 types of alkynes. Particularly, the introduction of well-dispersed Bi and PdC can induce prominent electron redistribution at the Pd−O4 sites and adjust the hybridization between the central Pd 3d and Bi 4f orbitals. Simultaneously, the strong electronic coupling in Pd−O−Bi pairs facilitated the d-electron domination near the Fermi level, boosted the activation of H2 and phenylacetylene at PdC sites, and improved the desorption capacity of styrene at Pd−O4 sites. This synergy ultimately lowers the energy barrier for the phenylacetylene semi-hydrogenation.
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PHYTOTHERAPY RESEARCH
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2026
·
IF 8.1
Lina Dong,Yuanxia Gao,Qian Li,Guangxin Chen,Dong Yang,Liping Zhao,Xiaojing Liu,Shumei Lin
Ulcerative colitis (UC) is a chronic inflammatory disease of the colon with limited effectiveness and safety of current drug therapies. Betulinic acid (BA) is a naturally occurring pentacyclic triterpenoid present in traditional Chinese medicines used clinically as retention enemas for UC, but its direct effects and mechanisms remain unclear. This study evaluated the therapeutic impact of BA enema in dextran sulfate sodium (DSS)-induced colitis by monitoring disease activity index (DAI), colon length, and histopathology, and by assessing inflammatory cytokines, mucosal tight junction, and mucin-2 (MUC2) expression. Colonic mucosa-associated microbiota were profiled by 16S rRNA gene sequencing. Potential BA targets were predicted using Swiss Target Prediction and validated by molecular docking, molecular dynamics simulations, cellular thermal shift assay, and biolayer interferometry. The functional relevance of the vitamin D receptor (VDR) was examined using a VDR antagonist in vivo and in vitro, and transcriptomic datasets from UC patients were analyzed to define VDR expression patterns. BA enema markedly attenuated DSS-induced colitis, such as reducing the DAI, inhibiting colonic damage, and improving colon length shortening. The BA also significantly restored the tight junction proteins, associated mucin proteins, and mucin-2 (MUC2). The BA reduced potentially pathogenic bacteria in the colonic mucosa. In addition, BA significantly restored the VDR proteins, and the VDR antagonist weakened the effects of BA in vivo and in vitro. The binding site between VDR and BA was Trp286. Transcriptomic analyses confirmed VDR downregulation in UC. These findings indicate that BA enema alleviates experimental colitis in part by targeting VDR to protect the intestinal mucosal barrier and modulate mucosa-associated microbiota, supporting BA as a promising candidate for UC treatment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Shiyi Huang,Hui Cao,Yongjun Lu,Fei-Fei Chen,Yan Yu
Developing efficient monolith catalysts for photocatalytic CO 2 reduction remains fundamentally challenging due to their inherently sluggish charge transfer. Herein, we report a Co 3 O 4 catalyst with serious agglomeration and meanwhile rich in oxygen vacancies (V O -r-Co 3 O 4 ), which achieves an unexpected superior photocatalytic CO evolution rate of 19.56 mmol h −1 g −1 . Experimental results and density functional theory (DFT) calculations reveal that V O play a crucial role in optimizing the CO 2 reduction pathway. Specifically, the abundant V O create a low-coordination environment around Co atoms, substantially weakening the Co O orbital hybridization. This directly induces a significant downshift of the Co 3 d -band center, effectively alleviating the overbinding of reaction intermediates. Consequently, the energy barriers for both the rate-determining *COOH formation and CO desorption are substantially reduced. This work highlights the importance of local electronic modulation in overcoming the charge transport limitations of monolith catalysts, offering a cost-effective strategy to revitalize such materials for solar energy conversion. Download: Download high-res image (146KB) Download: Download full-size image
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JOURNAL OF POWER SOURCES
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2026
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IF 8.4
Bowen Li,Haidong Xie,Hui Tian,Haojie Xu,Kaiyi Chang,Li Zhang,Chang Li,Jiao Hou,Xinwei Wang,Beiping Wang,Hui Lu,Shaolin Yang,Chunping Hou
Silicon suboxides (SiO x ) are promising anodes for lithium-ion batteries, but their practical application is hindered by severe volume fluctuation and sluggish (de)lithiation kinetics. Herein, a hierarchical disproportionated-SiO x -based composite, D-SiO x @NC/C@CNTs/rGO-2, consisting of disproportionated SiO x (D-SiO x ) with in situ generated Si/SiO 2 domains, a nitrogen-doped carbon/carbon (NC/C) interphase, and an interconnected CNTs/rGO conductive framework, is constructed through thermal disproportionation, interphase engineering, and multidimensional conductive-network design. Thermal disproportionation induces the in situ formation of Si domains embedded in a SiO 2 buffering matrix, in which Si provides lithium-storage activity while SiO 2 alleviates volume variation and enhances structural stability. Meanwhile, a conformal nitrogen-doped carbon interphase mitigates chemo-mechanical stress and stabilizes the active interface, and the intertwined CNTs/rGO framework builds an efficient conductive network. As a result, the optimized anode delivers a reversible capacity of 876.4 mAh·g −1 after 500 cycles at 0.5 A g −1 , with a capacity retention of 83.7%, while electrode swelling is suppressed to ≈52% versus ≈159% for bare D-SiO x . Operando electrochemical impedance spectroscopy combined with distribution of relaxation times reveals reduced interfacial polarization and faster apparent Li + transport. A pre-lithiated LFP||D-SiO x @NC/C@CNTs/rGO-2 full cell also shows an initial Coulombic efficiency of 96.15% and stable cycling over 200 cycles.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
·
IF 5.4
Zhongjian Wang,Guojun Lv,Jingbo Wang,Zhuoran Zhang,Yuhan Jiang,Yangbin Shen
The strong d-p covalent interaction of Mo-P bonds was obtained. • Lattice doping of P into MoS 2 formed Mo-P bonds in 0.2P-MoS 2. • 0.2P-MoS 2 achieved 91.7% tetracycline degradation under LED irradiation. Antibiotic pollution in water calls for sustainable remediation approaches such as photocatalysis. Despite its promising structure and visible-light response, MoS 2 is hindered by rapid carrier recombination, which severely restrict its photocatalytic efficiency. Herein, we reported a strategy of lattice phosphorus doping into MoS 2 to modulate the electronic structure, broaden visible-light absorption, and facilitate charge separation and migration. The optimized 0.2P-MoS 2 achieved 91.7% degradation of tetracycline (30 mg/L) within 80 min under low-power LED irradiation, with a reaction rate constant 5.5-fold higher than pristine MoS 2 . The superior photocatalytic degradation activity for 0.2P-MoS 2 arises from the narrowest band gap (1.21 eV) and accelerated charge carrier migration originated from the strong d-p covalent interactions in the generated Mo-P bonds. Radical scavenging experiments and electron paramagnetic resonance characterizations identified superoxide radicals (•O 2 − ) and holes (h⁺) as the dominant reactive species. Furthermore, possible photocatalytic degradation pathways of tetracycline were proposed over the 0.2P-MoS 2 catalyst. Moreover, the 0.2P-MoS 2 catalyst maintained high activity after five consecutive cycles, demonstrating its excellent stability. This work offers an electronic structure engineering perspective for rational design of MoS 2 -based photocatalysts and provides a viable approach for antibiotic degradation under low-power light sources, holding substantial promise for environmental remediation. Download: Download high-res image (187KB) Download: Download full-size image Strong d-p orbital hybridization of Mo-P bonds within phosphorus lattice-doped MoS 2 boosts visible-light photocatalytic degradation of tetracycline into CO 2 and H 2 O.
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BIOCHEMICAL AND BIOPHYSICAL RESEARCH COMMUNICATIONS
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2026
·
IF 2.5
Jing Wang,Xintong Chen,Yuanyu Tang,E. Pang,Duo Xia,Yongzhi Chen,Dan He,Kuansong Wang
Phototherapy has gained considerable attention in cancer treatment. Molecules with pronounced near-infrared (NIR) absorption are particularly advantageous for laser-induced phototherapy, as their NIR absorption enables deep tissue penetration while minimizing incidental damage to healthy tissues. In this study, we rationally designed and synthesized a non-fused ring A-D-A-type dye (T8IC4F) exhibiting both NIR absorption and fluorescence properties. Through self-assembly of T8IC4F with DSPE-PEG-NH 2 , water-dispersible nanoparticles (NPs) designated as C4@PEG were fabricated. The resulting C4@PEG NPs exhibit NIR absorption and NIR-II fluorescence properties and demonstrate significant therapeutic efficacy. Upon 808 nm laser irradiation (1 W·cm −2 ), these NPs exhibit a singlet oxygen ( 1 O 2 ) quantum yield of 25.9% and a photothermal conversion efficiency of 61%. These properties enable them to mediate both photodynamic and photothermal therapy, leading to robust antitumor efficacy. Moreover, C4@PEG NPs induce immunogenic cell death, facilitate the release of tumor antigens, and activate an antitumor immune response. These findings suggest that C4@PEG NPs could be applied in cancer phototherapy and immunotherapy.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2026
·
IF 6.7
Bo Zhang,Liqun Shen,Cheng Yu,Zhibo Leng,Zhihong Zhu,Lingfei Hua,Zijie Li
d-Allose, one of important rare sugars, has attracted increasing attention due to its low caloric value and remarkable physiological activities. l-Rhamnose isomerase (L-RI) catalyzes the reversible conversion of d-allulose to d-allose. However, its industrial application is limited by inadequate catalytic efficiency. In this study, L-RI from Clostridium thermosuccinogenes was identified and systematically characterized. Using a semirational protein engineering strategy, loop residues adjacent to the catalytic core and potential active sites predicted by the HotSpot Wizard web server were targeted. The resultant triple mutant N137Q/D258R/A265I achieved a d-allose conversion rate of 21.8% and a productivity of 130.8 g·L–1·h–1 within 1 h using 600 g·L–1 d-allulose. Molecular dynamics (MD) simulations revealed that modulation of loop flexibility enhanced the enzyme turnover rate. By fine-tuning loop flexibility while maintaining the structural integrity of the enzyme, this engineered mutant reduces the risk of enzyme inactivation during prolonged high-temperature catalysis. Collectively, these results highlight its potential for industrial d-allose production and provide valuable insights for the modification of L-RIs and related enzymes.
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PLASMA CHEMISTRY AND PLASMA PROCESSING
·
2022
·Vol. 43
·期 2
·491-511
·
IF 3.337
Huang Shaoyong,Huang Quanjia,Gan Jiaming,Li Ting,Wang Lei
In this study, Fe-rich sludge was pretreated by dielectric barrier discharge (DBD) and used as a Fenton catalyst for the degradation of 2,4-dichlorophenoxyacetic acid (2,4-D) in aqueous solution, where hydrogen peroxide was in situ supplied from a glow discharge plasma (GDP) in contact with the solution. Synergistic mechanism of the two plasmas during 2,4-D degradation was explored. The Fe-rich sludge pretreated by H 2 -DBD could significantly accelerate the 2,4-D degradation as it converted Fe(III) in the sludge to the active Fe(II). 2,4-D can be completely removed in the presence of H 2 -DBD pretreated Fe-rich sludge with 25 min of GDP at pH 0 3.0 and catalyst dosage of 1.0 g/L. Quenching experimental studies showed that both ·OH (oxidative degradation) and ·H (reductive dechlorination) were responsible for 2,4-D degradation. Reducing radicals (such as ·R and·H) formed during GDP can continuously reduce the Fe 3+ back to Fe 2+ , which further promoted the degradation and dechlorination of 2,4-D. The results of three consecutive experiments indicated the stability and reusability of catalyst. This study provides a potential method for the recycle of Fe-rich sludge as a novel and cost-effective catalyst for 2,4-D removal from aqueous environments, which is significant for the terminal disposal of Fe-rich sludge. Graphical Abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Sijia Liu,Xifei Zhou,Junxian Qin,Chaohai Wei,Yun Hu
Simultaneous redox reactions on photocatalysts make it possible to use wastewater for hydrogen production . The controlled synthesis of ultrasmall metal carbides effectively enhances the photocatalytic efficiency under this system. Here, we report a new type of cocatalyst in which a three-dimensional (3-D) nitrogen-doped carbon cage (NGC) of metal–organic framework derivatives encapsulates ultrasmall MoC nanoparticles (MoC@NGC), promoting simultaneous degradation of organic pollutants and hydrogen production by ZnIn 2 S 4 (ZIS). Characterization analyses showed that MoC accelerated the separation of the photogenerated carrier and effectively reduced the overpotential of hydrogen evolution , while NGC promoted the good dispersion of MoC particles and provided sufficient sites. The MoC@NGC/ZIS composite exhibited a high hydrogen (H 2 ) evolution rate of 1012 µmol g –1 h −1 , which exceed that of ZIS loaded with platinum. In the coupled system, where the electron donor was replaced with rhodamine B (RhB), the mechanism analysis showed that RhB and the as-generated intermediates consumed holes and facilitated hydrogen evolution. In addition, we designed a combined photocatalytic anoxic and oxic sequence process to achieve the recovery of hydrogen energy during the treatment of dye wastewater. This study provides a new way for cooperation between energy development and environmental protection.
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