ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yajie Guo,Fuxian Zheng,Ting Wang,Xinyang Liu,Xiaotan Tian,Konggang Qu,Lei Wang,Rui Li,Wenjun Kang,Zongge Li,Haibo Li
Palladium (Pd)-transition metal alloys have the potential to regulate the intermediate surface adsorption strength in oxygen reduction reactions (ORR), making them a promising substitute for platinum-based catalysts. Nonetheless, prolonged electrochemical cycling can lead to the depletion of transition metals, resulting in structural degradation and poor durability. Herein, the synthesis of alloy catalysts (Pd25%Te75%) containing Pd and the metalloid tellurium (Te) through a one-step reduction method is reported. Characterizations of powder X-ray photoelectron spectroscopy, X-ray diffraction, and high-resolution transmission electron microscopy demonstrated both uniform dispersion and strong binding force of elements within the PdTe alloy, along with providing crystallographic details of associated compounds. Based on density functional theory calculations, PdTe had a more negative d-band center than that of pure Pd, which reduces the adsorption capacity between active sites and intermediates in the ORR, and therefore enhances reaction kinetics. The Pd25%Te75% exhibited excellent ORR activity, and its onset and half-wave potentials were ∼0.98 and ∼0.90 V, respectively, at 1600 rpm within the O2-saturated 1.0 M KOH. Significantly, accelerated durability tests achieved exceptional stability, and half-wave potential just decayed by 4 mV after 30000 consecutive cycles. Moreover, this study aims to promote the preparation of Pd and metalloid alloys for other energy conversion applications.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xiaosong Zhou,Xiaoxing Yu,Lanzhen Peng,Jin Luo,Xiaomei Ning,Xuliang Fan,Xunfu Zhou,Xiaoqin Zhou
The photocatalytic H 2 production activity of polymer carbon nitride (g-C 3 N 4 ) is limited by the rapid recombination of photoelectron-hole pairs and slow surface reduction dynamic process. Here, a supramolecular complex (named R-TAP-Pd(II)) was fabricated via self-assembly of (R)-N-(1-phenylethyl)-4-(4-(pyridin-2-yl)-1H-1,2,3-triazol-1-yl)benzamide (R-TAP) with Pd(II) and used to modify g-C 3 N 4 . In the R-TAP-Pd(II)@g-C 3 N 4 composite photocatalyst, the spin polarization of R-TAP-Pd(II) can promote charge transfer and inhibit photogenerated carrier recombination, as confirmed by spectral tests and photoelectrochemical performance tests. Electrochemical tests and in situ X-ray photoelectron spectroscopy (XPS) tests proved that the Pd(II) ion in the R-TAP-Pd(II) molecule can serve as active sites to accelerate H 2 production. The R-TAP-Pd(II)@g-C 3 N 4 presented a photocatalytic H 2 generation rate of 1085 μmol g −1 h −1 when exposed to visible light, which was a about 278-fold increase compared with g-C 3 N 4 . This work finds a new approach to boost the photocatalytic efficiency of g-C 3 N 4 via supramolecular self-assembly.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Xi-Lai Liu,Wei Zhong,Yu-Fan Jin,Tian-Jiao Wang,Xue Xiao,Pei Chen,Yu Chen,Xuan Ai
The electrochemical hydrogenation (ECH) of 5-hydroxymethylfurfural (HMF) to 2,5-dihydroxymethylfuran (DHMF) represents a pivotal pathway for the electrocatalytic upgrading of biomass-based organic small molecules, offering significant reductions in energy consumption while producing value-added chemicals. The conversion of HMF to DHMF is challenging due to the high reduction potential and complex intermediates of HMF ECH under neutral environment. Also, the total efficiency is hindered by sluggish anodic oxygen evolution reaction (OER) kinetics. Herein, we report a synthesis of highly alloyed Pd-Pt bimetallene (Pd 3 Pt 1 BML) for HMF ECH coupled with formic acid oxidation reaction (FAOR). Through a combination of in-situ Raman spectroscopy, electron paramagnetic resonance analysis, and theoretical calculations, we elucidate that the HMF adsorption on Pd atoms, strategically separated by Pt atoms, is weakened compared to pure Pd surfaces. Additionally, Pt atoms serve as crucial providers of active hydrogen to neighboring Pd atoms, synergistically enhancing the reaction kinetics of HMF conversion with a Faradaic efficiency >93%. Meanwhile, the atomically dispersed Pt atoms endow Pd 3 Pt 1 BML with high electrochemical performance for the direct pathway of FAOR at the anode. As a result, a FAOR-assisted HMF ECH system equipped with bifunctional Pd 3 Pt 1 BML achieves the energy-efficient conversion of HMF to DHMF at electrolysis voltage of 0.72 V at 10 mA cm –2 . This work provides insights into the rational design of bifunctional catalysts featuring two distinct types of active sites for advanced energy electrocatalysis and ECH.
✓ 已验证
产品关联
DOI
高影响因子
Acta Pharmaceutica Sinica B
·
2024
·
IF 14.7
Jiaojiao Yu,Yujin Xiang,Yuzhen Gao,Shan Chang,Ren Kong,Xiaoxi Lv,Jinmei Yu,Yunjie Jin,Chenxi Li,Yiran Ma,Zhenhe Wang,Jichao Zhou,Hongyu Yuan,Shuang Shang,Fang Hua,Xiaowei Zhang,Bing Cui,Pingping Li
Protein kinase C α (PKC α ) regulates diverse biological functions of cancer cells and is a promising therapeutic target. However, clinical trials of PKC-targeted therapies have not yielded satisfactory results. Recent studies have also indicated a tumor-suppressive role of PKCs via unclear molecular mechanisms. In this study, we found that PKC α inhibition enhances CD8 + T-cell-mediated tumor evasion and abolishes antitumor activity in immunocompetent mice. We further identified PKC α as a critical regulator of programmed cell death-ligand 1 (PD-L1) and found that it enhances T-cell-dependent antitumor immunity in breast cancer by interacting with PD-L1 and suppressing PD-L1 expression. We demonstrated that PKC α -mediated PD-L1 phosphorylation promotes PD-L1 degradation through β transducin repeat-containing protein. Notably, the efficacy of PKC α inhibitors was intensified by synergizing with anti-PD-L1 mAb therapy to boost antitumor T-cell immunity in vivo . Clinical tissue array analysis revealed that PKC α expression is positively correlated with T-cell function and the interferon-gamma signature in patients with breast cancer. This study demonstrated the antitumor capability of PKC α , identified potential therapeutic strategies to avoid tumor evasion via PKC-targeted therapies, and provided a proof of concept for targeting PKC α in combination with anti-PD-L1 mAb therapy as a potential therapeutic approach against breast cancer, especially TNBC.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science Advances
·
2024
·Vol. 10
·期 36
·
IF 11.7
Mengjun Wang,Jun Jia,Zhaodong Meng,Jing Xia,Xinyan Hu,Fei Xue,Huiping Peng,Xiangmin Meng,Jun Yi,Xiaolan Chen,Jun Li,Yuzheng Guo,Yong Xu,Xiaoqing Huang
Photothermal catalysis effectively increases catalytic activity by using the photothermal effect of metal nanomaterials; however, the combination of strong light absorption and high catalytic performance remains a challenge. Here, we demonstrate hexagonal ~5-nanometer-thick palladium antimony (chemical formula as Pd8Sb3) nanosheets (NSs) that exhibit strong light absorption within full spectral and localized surface plasmon resonance (LSPR) effects in the visible region. Such LSPR features lead to strong photothermal effects, and Pd8Sb3 NSs aqueous dispersion enables enhanced photothermal methane (CH4) conversion to formaldehyde (HCHO) under full-spectrum light irradiation at 1.7 watts per square centimeter, leading to selectivity of ~98.7%, productivity of ~665 millimoles per gram of catalyst, ~700 times higher than that of Pd NSs. Mechanism investigations suggest that different radicals were generated on Pd8Sb3 (·OH) and Pd NSs (·O2−), where Pd8Sb3 NSs displays stronger adsorption strength to CH4 and facilitates CH4 oxidation to HCHO. Besides, the strong light absorption ability of Pd8Sb3 NSs enables photothermal therapy for breast cancer.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Energy and Sustainability Research
·
2024
·
IF 6.2
Seokyoung Hwang,Young Bean Hwang,Hyun Wook Hwang,Dansil Kim,Ji Young Lee,Jongkook Hwang,Eun Duck Park,Seok Ki Kim
This study investigates the mitigation of green oil deactivation in acetylene hydrogenation using carbon-supported Pd catalysts. Various carbon supports including CMK-3, short CMK-3, activated carbon, graphite, mesoporous carbon, graphite nanofiber, and carbon nanotube, are compared. Catalyst performance, including deactivation rates and product selectivity, is evaluated under high acetylene concentration conditions. Comprehensive characterization of catalyst properties is conducted using techniques such as scanning electron microscope, Ar physisorption, X-ray photoelectron spectroscopy, Raman spectroscopy, CO chemisorption, and thermogravimetric analysis. The study reveals that carbon-supported catalysts generally exhibit slower deactivation rates compared to alumina-supported catalysts. Among carbon supports, carbon nanotube demonstrates exceptional stability, while graphite shows rapid deactivation. The catalyst surface area shows the strongest correlation with the deactivation rate, suggesting that the larger the surface area, the easier it is for the generated green oil to escape without covering the active Pd sites. These findings highlight the importance of textural properties in designing stable catalysts for acetylene hydrogenation and emphasize the need for a holistic approach to catalyst design.
✓ 已验证
产品关联
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2024
·Vol. 137
·期 3
·1701-1720
·
IF 1.7
Guo Kailiang,Liu Shuang,Men Yong,Li Lin,Hu Jiajia,Xu Junzhe,Sun Chenghui,Wei Gaixia,Wang Jinguo,He Shan,Wu Bin,Huang Xiaohui
Herein, we prepared Pd nanoparticle (NP) catalysts using XC-72 carbon supports through a tailored deposition–precipitation method. Our primary objective was to unravel the size effects of Pd NPs on hydrogenation of tetraacetyldibenzylhexaazaisowurtzitane (TADBIW), a pivotal intermediate for synthesis of high energy density materials hexanitrohexaazaisowurtzitane (CL-20). The controlled modulation of Pd NP size ranged from a mere 1.8 nm to 7.4 nm. Remarkably, our investigations into TADBIW hydrogenation unveiled a fascinating trend: the ultrasmall-sized Pd NPs with a diameter of 1.8 nm exhibited excellent yield and reaction rates. In stark contrast, their larger-sized counterparts demonstrated diminished catalytic activities. To disclose the size-dependent nature, various characterization techniques were employed, including XRD, TEM, XPS, CO and H 2 pulse chemisorption. The comprehensive analysis revealed that the ultrasmall-sized Pd possessed more positively charged sites and exhibited higher dispersion. This unique configuration facilitated an accelerated adsorption of hydrogen and the electron-rich substrate TADBIW. Notably, this phenomenon led to a reduction in the activation energy through a thermodynamic effect, thereby enhancing overall catalytic performance. Our results strongly suggested that the ultrasmall-sized Pd NPs can exert a dominated influence on the physical and chemical states of the active sites, playing a key role in triggering the adsorption and activation of the substrate TADBIW. These findings not only deepen our understanding of the intricate connections between Pd NP size and catalytic activity but also open new avenues for advancing the design and optimization of catalysts in the hydrodebenzylation methodologies and synthesis of related compounds.
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Qiu Yu,Jiao Dongxu,Huang Hong,Wu Jiandong,Wang Mingming,Gao Tianyi,Zhao Xiao,Ge Xin,Zhang Wei,Zheng Weitao,Singh David J.,Fan Jinchang,Cui Xiaoqiang
Palladium hydride (PdH x ) metallenes are efficient electrocatalysts for the oxygen reduction reaction (ORR) due to their high atomic utilization and optimized oxygen binding energies modulated by interstitial hydrogen. However, their practical application is restricted by the highly unstable nature of interstitial hydrogen at working temperatures around 353 K. Here, we report that the use of Mn effectively locks hydrogen atoms within the Pd metallenes lattice, resulting in high alkaline ORR performance across a temperature range of 303–353 K. In contrast, the ORR activity of PdH x metallenes declines sharply with increasing temperature. At 353 K, the mass activity of PdMnH x metallenes at 0.95 V reaches 1.41 A mg − 1 , which is 14.1 times higher than that of PdH x metallenes. Multiple spectroscopic analyses and theoretical calculations reveal that strong electronic interactions within the immiscible Pd-Mn alloy are critical for locking interstitial hydrogen, thereby enhancing the ORR activity under high temperatures.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Meiling Chen,Xingyu Liu,Xiaole Weng,Renna Li,Zhongbiao Wu
The control of low-concentration methane (CH 4 ) emissions is a critical component of the ‘dual carbon’ strategy, and catalytic combustion technology focused on catalyst design is recognized as a promising avenue for achieving it. However, the zeolite-based catalysts are highly prone to deactivation under hydrothermal environments, thus limiting their practical applicability. Herein, we have utilized layered double hydroxides (LDHs) as precursors and integrated them with Pd/M through a co-precipitation method to fabricate Pd/M@CoAlO composite catalysts with a core–shell structure, focused on the impact of CoAlO morphology on the activity and stability for CH 4 oxidation. It revealed that the incorporation of CoAlO significantly enhanced the catalytic combustion efficiency and the hydrothermal stability of Pd/M. Furthermore, an increase in the calcination temperature led to a progressive degradation of the sheet-like or petal-shaped structure of CoAlO within the Pd/M@CoAlO composite catalysts. This structural collapse eventually resulted in the formation of CoAlO dense particles that enveloped the Pd/M, adversely affecting the adsorption of oxygen and the exposure of active sites. This work underscores the importance of morphological control, providing significant guidance for the strategic design and development of catalysts tailored for CH 4 catalytic combustion.
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
·
2025
·
IF 14.1
Manman Tan,Chengyu Shi,Guangyi Chi,Xinwan Su,Fangzhou Liu,Linyu Zhu,Guangqian Cheng,Xiangyi Chen,Meng Yu,Yijian Chen,Ying Wang,Yu Chen,ShuLing Yan,Wenfei Wu,Qingfeng Yan,Jianzhong Shao,Kai Wang,Xiangrui Liu,Min Zhou,Aifu Lin
Peptide-based therapeutic strategies offer considerable potential for tumor immunotherapy but suffer from poor systemic bioavailability, rapid plasma clearance, and limited tumor-targeting efficiency. To address these challenges, a biomimetic, photothermal-responsive liposomal delivery system was developed that enables precise delivery of immunotherapeutic peptides while enhancing the synergistic effects of photothermal therapy. This system enhances peptide stability through fluorination, disrupts post-translational modifications of PD-L1, and promotes its degradation, thereby amplifying the anti-tumor immune response. The carrier core consisted of thermosensitive 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC) liposomes loaded with the low-toxicity photosensitizer indocyanine green (ICG), which facilitated controlled peptide release via the photothermal effect. Simultaneously, mild photothermal stimulation induced immunogenic cell death (ICD), further strengthening anti-tumor immunity. To enhance tumor targeting, extend systemic circulation time, and improve drug accumulation at tumor sites, the carrier surface was coated with a platelet membrane, which increased biocompatibility and promoted immune evasion. Notably, in vivo studies demonstrated that the developed bioengineering platform significantly suppressed tumor growth in both solid and diffuse malignant tumors while inducing persistent immune memory, thereby facilitating long-term anti-tumor immune responses. Collectively, this approach establishes a novel framework for integrating peptide drug delivery with photothermal therapy, offering a promising strategy for advancing tumor immunotherapy.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
npj Precision Oncology
·
2025
·Vol. 9
·期 1
·1-15
·
IF 8
Huo Ran,Xu Quan-guo,You Yi-qing,Chen Yan-lin,Su Guang-jian,Yang Kun-rong,Xiao Yan-ping,Xue Zhong,Li Yang-jin,Sun Pei,Cui Zhao-lei,Lin Ying-ying,Guo Jun-ying,Xu Hai-yan,Chen Zhao-shuo,Xie Wen-ting,Xu Shao-hua,Chen Min-yong,Wu Jing,He Shi-jie,Xiao Zhen-zhou,Chen Yan
Hepatocellular carcinoma (HCC) is a prevalent and deadly cancer. Gut microbiota affect tumor immunity and immunotherapy efficacy, but the exact mechanisms are unclear. A study compared gut microbiota in HCC patients and healthy controls (HC) using 16S rDNA analysis and metabolomics. It found higher levels of Bifidobacterium and a positive correlation between Bifidobacterium and isobutyric acid in HC group. Animal models showed that the combination of HC fecal matter and αPD-1 treatment reduced tumor volume more effectively than the combination of HCC fecal matter and αPD-1. The combination of Bifidobacterium or isobutyrate with αPD-1 also decreased tumor size. In vitro, isobutyrate-stimulated CD8 + T cells increased IFN-γ secretion, suppressed liver cancer cells, and downregulated the JAK/STAT3 pathway. Combined treatments increased CD8 + T cells and IFN-γ levels and reduced JAK/STAT3 signaling in the tumor microenvironment. This suggests that Bifidobacterium and isobutyrate can inhibit tumor growth, offering insights into gut microbiota-host interactions and potential strategies to overcome HCC immunotherapy resistance.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-8
·
IF 15.7
Deng Peilin,Xu Yueshan,Wu Daoxiong,Liang Ying,Zhang Xue,Wang Zhitong,Li Jing,Tian Xinlong
Pd catalysts demonstrate remarkable activity and selectivity for the direct oxidation methane-to-methanol (DOMM) under mild conditions. However, understanding the structure–performance relationship is challenging because Pd catalysts used in existing studies have complex polycrystalline structures. In this work, well-defined Pd nanocrystals with controlled morphologies are synthesized and used as model systems to investigate the origins of the observed structure-activity differences. Our findings indicate that DOMM activity is primarily governed by crystal facet type rather than nanocrystal size. The lower d -band center of the Pd {111} facet weakens the adsorption strength of critical intermediates, including *O 2 and *OH species, promoting H 2 O 2 generation and CH 3 OH formation, respectively. Consequently, {111}-dominated octahedral Pd nanocrystals achieve an exceptional CH 3 OH yield of 201.8 mmol·g Pd −1 ·h −1 , three times higher than that of their {100}-dominated hexahedral counterparts. These results provide key insights into the structure-dependent behavior of Pd catalysts and pave the way for designing high-performance catalysts for DOMM.
✓ 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）