ChemSusChem
·
2026
·Vol. 19
·期 16
·e70987
·
IF 5.9
Wenguang Li,Penghui Li,Shubin Wu,Xiaohui Wang
Kraft lignin, an abundant renewable aromatic polymer, has attracted increasing interest for acid‐catalyzed depolymerization to obtain lignin oil with high antioxidant activity. However, this process is plagued by severe condensation of reactive intermediates, leading to low lignin oil yields. To address this critical issue, we performed preacetylation modification on hardwood kraft lignin (HKL) and investigated its depolymerization behavior in acidic deep eutectic solvents (DESs). Furthermore, the underlying mechanism by which acetylation promotes depolymerization was clarified using lignin monomer model compounds. The results demonstrated that acetylation effectively increased the lignin oil yield. Specifically, at a degree of substitution (DS) of 66.57% (AHKL‐20), the lignin oil yield increased markedly from 37.80% to 55.98%. Additionally, lignin oil derived from AHKL‐20 (lignin oil AHKL‐20 ) exhibited higher antioxidant capacity (IC 50 = 5.18 μg/mL) than HKL (IC 50 = 13.02 μg/mL). This study proposes a novel strategy based on the structural premodification of kraft lignin to inhibit condensation, enabling efficient and mild depolymerization in green solvents. Preacetylation shields active hydroxyl groups of kraft lignin, suppressing undesired condensation during acid‐catalyzed depolymerization and thereby increasing lignin oil yield.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEDICINAL CHEMISTRY
·
2026
·
IF 6.8
Xinyue Zhao,Naijie Wei,Ziyang Fang,Yingyan Xie,Xiaowen Yan,Qiuquan Wang
To address the low cytotoxicity and drug resistance issues of targeted covalent inhibitor (TCI) ibrutinib and severe side effects of chemotherapeutics doxorubicin (DOX), we developed a novel targeted covalently activated chemotherapy strategy. We designed and synthesized a targeted covalently activated chemotherapy drug, Ibt-DOX, which features a targeting ligand of ibrutinib, a DOX, an electrophilic warhead α-methylated acrylamide (α-MAA) and a self-immolative linker p-hydroxybenzyl alcohol. Upon specifically binding to BTK, Ibt-DOX inhibits the BTK-mediated BCR signaling, meanwhile releases DOX and induces immunogenic cell death (ICD), ultimately resulting in not only significantly enhanced targeted B-cell lymphoma cells death compared with ibrutinib, but also reduces the toxic side effects of DOX on BTK- cells. Our work offers a novel strategy through leveraging the synergistic effect of targeted covalent inhibition and the high cytotoxicity of chemotherapy drug, which will inspire the development of new targeted covalent chemotherapeutics for different cancers treatment.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Haiyang Xie,Yuhan Chen,Xianni Li,Xiaoling Lu,Hao Lin,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Tao Gan
The selective oxidation of benzyl alcohol (BzOH) to benzaldehyde (BzH) is one of the effective methods for synthesizing chlorine-free benzaldehyde, but developing an efficient catalytic system remains a challenge. The peroxymonosulfate (PMS) is an inexpensive and soluble solid oxidant that has been widely used in oxidation reactions in aqueous media, however, there are still difficulties in activating PMS using atomically dispersed metal catalysts based on non-free radical pathways. Herein, an atomically dispersed manganese catalyst (Mn 1 /NLC), featuring electron-deficient Mn–N 2 O 2 sites anchored on a nitrogen and oxygen co-doped carbon support, is synthesized through a combined process of ball milling and high-temperature pyrolysis. The Mn 1 /NLC catalyst exhibits outstanding performance in the selective oxidation of BzOH to BzH by efficiently activating PMS, achieving 98.5% BzOH conversion and 99.2% BzH selectivity with a high turnover frequency of 1470.6 h −1 within 3 h at a PMS dosage of 10 mg and 45 °C, which surpasses the majority of the reported catalysts. Electron paramagnetic resonance, radical quenching experiments, and electrochemical analysis collectively reveal that the Mn–N 2 O 2 reaction sites lead to the formation of a high-valent Mn species, which enhances the adsorption of C H bonds and activation of PMS to significantly promote the occurrence of non-radical oxidation pathway, including singlet oxygen ( 1 O 2 ) generation and electron transfer processes (ETP). The synergistic effect of 1 O 2 and ETP enables Mn 1 /NLC to perform efficient and selective C H oxidation of various aromatic alcohols under mild conditions, while also demonstrating excellent cycling stability. This study provides a novel strategy for the design of high-performance atomically dispersed metal catalysts for the selective oxidation of aromatic alcohols.
✓ 已验证
产品关联
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2026
·
IF 9
Tianyin Huang,Yifan Yu,Wentao Zhang,Yue Zhao,Yiliang Tao,Wenguang Huang,Bingdang Wu
Antibiotic residues, as emerging environmental contaminants, have raised significant concerns, underscoring the urgent need for efficient laccase–mediator systems (LMS) to facilitate their removal. However, the screening and design of high-performance mediators remain largely empirical, lacking robust theoretical guidance. In this study, we systematically evaluated the kinetic performance of Trametes versicolor laccase coupled with 19 redox mediators for sulfamethoxazole (SMX) degradation in the presence of humic acid (HA). Among the mediators tested, syringaldehyde (SA) exhibited superior degradation efficiency. By promoting laccase-catalyzed generation of phenoxyl radicals, the kinetics of antibiotic removal was improved. Toxicity assessments revealed that the degradation products of SMX in the SA-mediated LMS with HA exhibited low ecological risk. The system maintained high SMX degradation performance in various real water matrices (with a removal rate of up to 95 % and a reaction rate of up to 0.11 min −1 ), demonstrating its applicability in environmentally relevant scenarios. Furthermore, we established a structure–activity relationship between the electronic properties of natural mediators and SMX removal efficiency, demonstrating that catalytic performance is closely correlated with frontier molecular orbital energy levels and HOMO (Highest Occupied Molecular Orbital)–LUMO (Lowest Unoccupied Molecular Orbital) gaps. High-efficiency mediators typically possess higher HOMO energies and narrower energy gaps. This study offers molecular-level insights and design principles for developing efficient mediators, advancing the targeted application of LMS technology for the remediation of emerging contaminants.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Forests
·
2026
·Vol. 17
·期 8
·956
·
IF 3.1
Yong Wang,Yongyao Li,Zhongjun Cheng,Caiyun Wang,Min Liu,Maochang Zhou,Xiangyu Zhang
Under-forest wild-simulated cultivation ofGastrodia elataBl.f. glauca S. Chow(Wu Tianma, WTM) offers a viable pathway for reconciling ecological conservation with economic and health benefits, yet optimal seed tuber regimes remain understudied. We established nine planting regimes varying in single-tuber weight and per-hole dosage in a karst plateau area, monitored tuber yield and bioactive components (gastrodin,p-Hydroxybenzyl alcohol, and parishin), and evaluated performance via one-way ANOVA and a comprehensive index. At equal per-hole dosage, individual tubers of 10–15 g achieved the highest comprehensive index (57.13%), whereas those <5 g performed poorly (28.66%). With respect to seeding rate, the maximum yield (5.27 kg/m2) was achieved at 250 g per hole, while the highest combined content of gastrodin andp-Hydroxybenzyl alcohol (0.29%) and the peak parishin content were observed at 350 g and 150 g per hole, respectively. While tuber weight and seeding rate significantly affected yield, they had minor impacts on bioactive composition, suggesting that medium-sized seed tubers with moderately increased dosage can synergistically improve yield and quality. Our findings provide empirical benchmarks for germplasm selection and agronomic optimization in WTM cultivation, and call for multi-scale studies integrating soil microbiota and microclimate to unravel cascading mechanisms for sustainable quality enhancement.
✓ 已验证
产品关联
DOI
高影响因子
BIOMATERIALS
·
2022
·
IF 15.304
Hongjie Zhang,Weijian Chen,Jing Wang,Wenxiang Du,Bibo Wang,Lei Song,Yuan Hu,Xiaopeng Ma
Reactive oxygen species (ROS) as well-known endogenous stimuli has been widely used to activate drug delivery systems (DDSs) for tumor-specific therapy. Unfortunately, endogenous ROS in the tumor microenvironment (TME) is not enough to achieve effective therapeutic efficacy and cancer cells have adapted to high oxidative stress by upregulating glutathione (GSH) level. Herein, we devised a novel ROS-activable self-immolative prodrug CASDB with both GSH-depletion ability and ROS self-supply competence. Then, an stimuli-responsive nanoplatform integrating CASDB with clinical chemotherapeutics mitoxantrone (MTO) and PLGA was fabricated (denoted as CMPs) through nanoprecipitation method. The CMPs could achieve desired accumulation at tumor tissues through enhanced permeability and retention (EPR) effects. Then the accumulated CMPs could induce tumor cell apoptosis efficiently. Especially, ROS in tumor sites could trigger the immolation of CASDB to generate CA and quinone methide (QM). Then CA and QM cooperatively promoted damage of mitochondria due to oxidative stress and led to cancer cells more sensitive to MTO. Accordingly, MTO could perturb cellular microenvironment of cancer cells then promote the degradation of CASDB. The experiment results demonstrated that CMPs were ideal for desirable synergetic tumor-specific anticancer therapy with negligible systemic toxicity. The half-maximal inhibitory concentrations (IC50) value of CMPs was 6.53 μM, while the IC50 values of MTO was 14.76 μM. And the CMPs group showed the strongest tumor suppressor effect with the tumor sizes increased to 1.2-fold (Control group: 20.6-fold, MTO only: 3.0-fold). This study should be inspirational for designing efficient prodrugs to overcome the handicaps of traditional chemotherapy.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2023
·
IF 7.4
Xingjie Guo,Peng Hong,Lu Yao,Xudong Liu,Zhicheng Jiang,Bi Shi
Selective conversion of lignin derivatives into value-added chemicals benefits to develop sustainable chemical engineering and material manufacturing. In this work, a hydrotalcite-supported PdNi bimetallic catalyst was synthesized by introducing Ni to promote Pd dispersion and adjust the charge distribution of the active center, which was used for the catalytic hydrogenation of lignin-derived aldehydes in water under mild conditions. At 30 ℃ and 2 MPa H 2 , PdNi/HT achieved 99 % of vanillin (VAN) conversion with 100 % selectivity of vanillyl alcohol (VAL), and most of the typical lignin-derived aldehydes could be hydrogenated over this catalyst. This catalyst was steady and could be recycled at least five runs. The introduction of Ni and the nanosheet structure of HT improved the dispersion of the metal particles, significantly reducing the metal particle size. Besides, the Pd δ− –Ni δ+ pair and the basic sites of HT facilitated the H 2 activation and the adsorption of the aldehyde groups of lignin-derived aldehydes on the catalyst surface, enhancing the hydrogenation efficiency and selectivity.
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2023
·
IF 5.3
Zhenyu Li,Enhui Du,Panpan Hao,Liyuan Huai,Yang Zhong,Soliman I. El-Hout,Chunlin Chen,Jian Zhang
The oxidation of biomass-derived 5-hydroxymethyl furfural (HMF) into 2,5-Furandicarboxylic acid (FDCA) is a favorable reaction since FDCA is an ideal alternative to petroleum-based monomer terephthalic acid in bio-based polyester industry. However, producing FDCA with high yield under mild conditions is still challenging, especially at energy-saving near-ambient temperatures. Here, we present a Pd nanoparticles catalyst supported on Vulcan XC-72 carbon (Pd/VC) that can completely convert HMF and achieve an encouraging FDCA yield (92.4%) at 30 ℃. The most important observations include yield declines at pure oxygen bubbling, and the transformation of intermediates becomes stagnant; instead, switching to the diluted oxygen is effectively driving the tandem oxidation as the over-oxidation, and thus, rapid deactivation of the Pd surface could be alleviated. The negative effect of high oxygen concentration also occurs in the dehydrogenation and oxygenation of an extended substrate. Since the decisive influence of oxygen content has often been neglected in past investigations of oxidative transformation over Pd-based catalysts, the current study may offer a critical reminder for other liquid-phase oxidation reactions.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
·
IF 8.025
Peng Xie,Wang Zhang,Wugao Wu,Zhuanglin Shen,Mingliang Wang,Yuxiao Lai,Yantao Chen,Zhongfan Jia
A mediation strategy can effectively overcome the low reaction activity of enzymes with nonspecific substrates. In this study, we demonstrated how phenol compounds can mitigate the substrate limitation of HRP in catalytic degradation of various organic pollutants. In a classical HRP/H 2 O 2 system, phenol and natural phenolic compounds (4-HBA & pHBA), exhibited up to over 100-fold enhancement in eliminating organic dyes and persistent antibiotics while the loading is only 2–5 wt%. A combination of molecular modelling, docking and frontier orbital energy analysis was employed to elucidate the catalytic performance and mechanism. We revealed that (1) generating phenoxyl radicals required the proximity of mediators to the HRP active centre, and (2) the subsequent efficient radical transfer to pollutants was determined by the large energy gap between the SOMO energy of phenoxyl radicals and the HOMO energy of phenols. When considering phenols as pollutants, we showed a synergistic effect on catalytic degradation of phenols, dyes, and tetracycline with a removal efficiency of 71–92 %. Overall, this work not only demonstrates that phenoxyl mediators can overcome the lower efficiency and substrate-specificity limitations of the HRP/H 2 O 2 system but also revealed their structure-mediation relationship, implying great potential in the biodegradation of diverse pollutants and their mixtures.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today
·
2022
·
IF 26.943
Yue Wei,Si Wu,Zhenqi Liu,Jingsheng Niu,Ya Zhou,Jinsong Ren,Xiaogang Qu
Cancer immunotherapy has emerged as a promising cancer treatment. However, its efficacy is often limited by the immunosuppressive tumor microenvironment (TME) in solid tumors. Herein, a new strategy has been presented by using bioorthogonal chemistry to reprogram TME. We designed a bifunctional mannose (Man) vector decorated palladium bioorthogonal nanozyme for in-situ synthesis of histone deacetylase inhibitor (HDACi) vorinostat (FDA approved) with the ability to remodel tumor microenvironment. To the best of our knowledge, this is the first report to use a bioorthogonal nanozyme for cancer immunotherapy. In particular, the nanozyme could preferentially accumulate in M2 macrophages (termed M2Φ) to achieve local M2 re-education, which effectively avoided unnecessary inflammation in normal tissues. Moreover, vorinostat-induced TME reprogramming was synergistic with peroxidase-like activity of the nanozyme, and achieved enhanced tumor synergistic immunotherapy. In colon cancer (CT26)-tumor-bearing BALB/c mice, the nanozyme demonstrated macrophages polarization targeting M2Φ and activation of innate immune system, resulting in significantly enhanced tumor growth inhibition. Our work not only provides a new effective way to reprogram TME in vivo, but also shed light on the design of novel bioorthogonal nanozymes for cancer immunotherapy.
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2023
·
IF 9.8
Zixin Xie,Xihong Zu,Jinxin Lin,Xueqing Qiu,Tengda Liang,Liheng Chen
The biomass flow fuel cell (BFFC) is a promising technology for realizing a sustainable society. However, BFFCs generally require electron mediators and complex pretreatment, resulting in miscellaneous ion pollution and energy consumption. Herein, we develop a lignin flow fuel cell (LFFC) for self-generating electricity via the privileged structure and redox chemistry of lignin without any electron mediators and pre-reaction. The experiments and theoretical simulations reveal that lignin can automatically release electrons by its oxidation and cleavage under a high voltage difference to achieve high cell performance. Interestingly, phenolic lignin model compounds with more methoxy groups exhibit higher cell performance because the methoxy groups can significantly reduce their HOMO–LUMO energy gaps and oxidation potentials, which is beneficial for releasing electrons. When industrial lignin was utilized as the fuel, the LFFC achieved a high power density of 159.9 mW cm−2 and worked stably for more than 8 h with 5.0 g lignin. Moreover, the LFFC fueled by 1.0 g lignin can output 219.9 mW h electrical energy, which is significantly higher than that of the reported BFFCs. Furthermore, the scale-up of the LFFC can power several electrical devices simultaneously at room temperature. This work provides a promising approach for next-generation LFFCs with low cost and high performance towards a sustainable future.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Peng Zeng,Wei-De Zhang
Evolution of hydrogen from water by utilizing solar energy and photocatalysts is one of the most promising ways to solve energy crisis. However, designing a cost-effective and stable photocatalyst without any noble metals is of vital importance for this process. Herein, an extremely active molecular complex cocatalyst NiL 2 (Cl) 2 is successfully designed. After being covalently linked to thiophene-embedded polymeric carbon nitride (TPCN), the hybrid catalyst NiL 2 (Cl) 2 /TPCN exhibits extraordinary H 2 production activity of 95.8 μmol h −1 without Pt (λ ≥ 420 nm), together with a remarkable apparent quantum yield of 6.68% at 450 nm. In such a composite catalyst, the embedded π-electron-rich thiophene-ring not only extends the π-conjugated system to enhance visible light absorption, but also promotes the charge separation through electron-withdrawing effect. It turns out that the C N covalent bonds formed between NiL 2 (Cl) 2 and TPCN skeleton accelerate the transfer of electrons to the Ni active sites. Our finding reveals that the strategy of embedding π-electron-rich compounds to graphitic carbon nitride provides potentials to develop excellent photocatalysts. The strong covalent combination of molecular complexes cocatalyst onto organic semiconductors represents an important step towards designing noble-metal-free photocatalysts with superior activity and high stability for visible light driven hydrogen evolution .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）