ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Xiaoyu Shi,Yang Yang,Xin Ye,Heng Zhong,Chunling Wang,Fangming Jin
Catalytic conversion of cellulosic biomass into polyols is an effective approach for biomass upgrading. However, the conversion involves cascade reactions which require various catalytic sites cooperation for activating specific steps, resulting in low efficiency. Here, we propose a bifunctional catalyst containing acid sites and hydrogenation capacity for polyol production with cellobiose as the model compound of cellulose. Phosphonic acids (PAs) containing either methyl (MPA) or aminomethyl (NH2MPA) tails were used to tune the Pd/Al2O3 catalyst to form monolayers, thereby modulating the surface physiochemical properties and introducing multiple catalytic sites. An increasing ratio of PdO/Pd and a strong metal–support interaction were observed after PA modification, which could boost the hydrogenation activity for cellobiose. Furthermore, Pd/Al2O3-MPA exhibited excellent hydrolytic hydrogenation activity due to the increase of Lewis acid sites with good durability under hydrothermal conditions by MPA modification, achieving a 78.5% yield of sorbitol at 180 °C for 5 h. A plausible mechanism for enhancing the synergistic effect of Pd and support over Pd/Al2O3-MPA was also proposed. This investigation provides a novel strategy for rationally designing hydrothermally stable bifunctional catalysts to utilize biomass in a more effective way.
研究领域:
催化化学
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生物质能
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产品关联
DOI
高影响因子
AICHE JOURNAL
·
2023
·Vol. 69
·期 7
·e18078
·
IF 3.7
Yanping Yang,Jiarui Yang,Shucheng Shi,Yunhong Luo,Xingjun Xu,Yanan Liu,Dianqing Li,Junting Feng
Selective acetylene hydrogenation is a strongly exothermic process, easy to cause coking and metal agglomeration, and thus leads to deactivation. In this work, Pd/TiO 2 with different oxygen vacancies (V o ) were synthesized by controlling reduction temperature in 300–700°C, in which Pd/TiO 2 -HT300 (HT is reduction temperature) possessed the highest V o content. It was found highly dispersed Pd nanoparticles adjacent to more V o exhibited enhanced catalytic behavior (near 100% conversion at 55°C with 80% selectivity and turnover frequency of 0.12 s −1 ) due to hydrogen spillover generation and electron donation originating from V o sites, confirmed by in situ x-ray photoelectron spectroscopy, in situ Raman, and H 2 -temperature programmed desorption. More importantly, the increasing V o sites trap the released heat and devote to a decrease of heat accumulation over a single active Pd site, and consequently inhibit Pd agglomeration and polymerization, affirmed by high-resolution transmission electron microscopy, CO chemisorption, and thermogravimetric analysis.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Yinan Wang,Xuteng Zhao,Ting Chen,Zuwei Zheng,Rijing Zhan,He Lin
Pd/SSZ-13 with different Al distributions were hydrothermally synthesized and utilized as passive NOx adsorbers (PNA). The characterization results indicated that more concentrated Al distribution can not only improve the ion-exchanged level of Pd but also generated more Z 2 Pd 2+ sites at six-member rings. Thus, as revealed by NOx adsorption experiments, samples with more Z 2 Pd 2+ sites showed high NOx storage capacity as well as stronger water resistance. Besides, 84.8 % adsorption capacity of this sample was retained after hydrothermal aging treatment. On the other side, Pd existed as [Pd(OH)] + sites on SSZ-13 with isolated Al as the majority. These sites were vulnerable to H 2 O and less stable. Seriously Pd agglomerated was observed on the aged Pd/SSZ-13 with less paired Al. This study revealed that proper Al distribution on SSZ-13 could significantly improve the performance and stability of the catalyst and provided a new direction for the design of PNA catalysts.
研究领域:
催化化学
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环境科学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Wen Li,Kuncan Wang,Guowu Zhan,Jiale Huang,Qingbiao Li
The chemical transformation of CO2 to value-added chemicals and fuels remains a daunting research challenge, requiring the development of more efficient catalysts. The present work offers highly active integrated nanocatalysts for CO2 hydrogenation to dimethyl ether (DME) through tandem catalysis, that is, Pd/ZnO converts CO2 to methanol, and bio-ZSM-5 further catalyzes methanol dehydration to DME. Notably, the hierarchically porous bio-ZSM-5 with high pore connectivity was prepared by using low-cost rice husk and luffa sponge as biotemplates. The formation of bio-ZSM-5 involved three consecutive steps, including (i) diffusion of precursor species, (ii) confined crystal growth, and (iii) calcination treatment to remove the residual biomass. Interestingly, the obtained bio-ZSM-5 possesses abundant hierarchical porosity, including the intrinsic micropores from ZSM-5 frameworks, the mesopores from intracrystalline void space or pinholes in the intergrown zeolite layers, and the macroscopic channels from the original biomass architecture. It was found that the tetrapropylammonium hydroxide amount and Si/Al ratio were two critical factors affecting the crystallinity and porosity of the bio-ZSM-5. The silicon content in biomass (8.3 wt % in rice husk and 0.016 wt % in luffa sponge) also played a crucial role in the synthesis of bio-ZSM-5. Different spatial configurations of Pd/ZnO and bio-ZSM-5 significantly affected the DME yield, wherein spatial distances between the bio-ZSM-5 and Pd/ZnO components were adjusted by controlling the size of Pd/ZnO or the integration manners. The current results indicated that the closest proximity of the bifunctional catalyst was unfavorable for DME production (selectivity < 3%), because of which low-valent Zn cations from Pd/ZnO could displace the Brønsted acid sites on bio-ZSM-5 by ion exchange, and the powder mixing in the mortar was the best combination configuration of Pd/ZnO and bio-ZSM-5, promoting the CO2 conversion (10.8%) with a DME selectivity of 31% under the reaction of 300 °C and 30 bar. Furthermore, as compared to the traditional ZSM-5 based catalyst, the obtained Pd/ZnO/bio-ZSM-5 bifunctional catalysts showed excellent long-term stability in 60 h on stream with a less amount of coke formed in the spent catalysts.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
ChemCatChem
·
2023
·Vol. 15
·期 7
·e202300194
·
IF 4.5
Tao Li,Mengling Dong,Jiacheng Xu,Tiantian Zhang,Yan Sun,Ning Li,Zuliang Wu,Jing Li,Erhao Gao,Jiali Zhu,Shuiliang Yao,Yong Huang
Graphical CeO 2 /γ-Al 2 O 3 , Pd/CeO 2 , and Pd/CeO 2 /γ-Al 2 O 3 were used for catalyzing low-concentration CH 4 oxidation . γ-Al 2 O 3 can efficiently promote CH 4 oxidation on Pd/CeO 2 and the formation of bicarbonate that is easily gasified to CO 2 . CeO 2 /γ-Al 2 O 3 , Pd/CeO 2 , and Pd/CeO 2 /γ-Al 2 O 3 were used for catalyzing low-concentration CH 4 oxidation. It was found that nano-sized Pd could obviously promote CH 4 oxidation on CeO 2 /γ-Al 2 O 3 . The interaction between Pd and CeO 2 on γ-Al 2 O 3 resulted in higher ratios of Ce 3+ /(Ce 3+ +Ce 4+ ), Pd 2+ /(Pd 2+ +Pd δ+ ), and O ads /(O ads +O latt ), those benefited the formation of more oxygen vacancies and surface reactive oxygen species for CH 4 oxidation. γ-Al 2 O 3 not only supplied a high surface area and enhanced Pd/CeO 2 dispersion on γ-Al 2 O 3 , but also simulated the formation of bicarbonate, where bicarbonate is easier to gasify to CO 2 than bidentate carbonate that formed on Pd/CeO 2 . Operando diffuse reflectance infrared Fourier transform spectroscopy-mass spectrometer analysis results showed that CH 4 oxidation could occur at a temperature as low as 180 °C due to the reaction with surface reactive OH, this reaction was also accompanied by the formation of bicarbonate. The mechanism of CH 4 oxidation promoted by bicarbonate formation on γ-Al 2 O 3 was proposed.
研究领域:
催化化学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2024
·
IF 1.5
Xu Xiang,Mao Yiyin,Zhou Peng,Wu Yujing,Liu Yaling,Wang Hongyong,Lu Chunxiong,Zou Pei
In this study, a 99m Tc-labeled small molecule imaging probe [ 99m Tc]Tc-PG3C-CBM for PD-L1 imaging was designed. It showed a radiochemical yield of > 97% and good in vitro stability. Uptake in A375-hPD-L1 cells (17.07 ± 1.40%) was 4.5 times higher than in A375 cells (3.81 ± 0.19%). The probe demonstrated moderate PD-L1 affinity (K D : 11.6 ± 2.57 nM; IC 50 : 59.2 ± 2.40 nM). Additionally, SPECT/CT imaging and biodistribution results indicated that [ 99m Tc]Tc-PG3C-CBM was mainly metabolized by the liver and showed some accumulation at the tumor site. These results suggest that [ 99m Tc]Tc-PG3C-CBM could potentially target PD-L1 at tumor sites.
研究领域:
核医学
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分子影像学
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肿瘤学
✓ 已验证
DOI
高影响因子
Acta Biomaterialia
·
2021
·
IF 8.947
Zefeng Wang,Yanling Peng,Yan Zhou,Shengnan Zhang,Jianxi Tan,Huan Li,Dinggeng He,Le Deng
Photothermal therapy (PTT) is a promising strategy for antimicrobial therapy. However, the application of PTT to treat bacterial infections remains a challenge as the high temperature required for bacterial elimination can partly damage healthy tissues. Selecting the appropriate treatment temperature is therefore a key factor for PTT. In this work, we designed a near-infrared/pH dual stimuli-responsive activated procedural antibacterial system based on zeolitic imidazolate framework-8 (ZIF-8), which was bottom-up synthesized and utilized to encapsulate both Pd-Cu nanoalloy (PC) and the antibiotic amoxicillin (AMO). This procedural antibacterial therapy comprises chemotherapy (CT) and PTT. The former disrupts the bacterial cell wall by releasing AMO in an acidic environment, which depends on the sensitive response of ZIF-8 to pH value change. With the progression in time, the AMO release rate decreased gradually. The latter can then significantly stimulate drug release and further complete the antibacterial effect. This impactful attack consisted of two waves that constitute the procedural therapy for bacterial infection. Accordingly, the treatment temperature required for antibacterial therapy can be significantly lowered under this mode of treatment. This antibacterial system has a significant therapeutic effect on planktonic bacteria (G + /G − ) and their biofilms and also has good biocompatibility; thus, it provides a promising strategy to develop an effective and safe treatment against bacterial infections. Statement of Significance We have developed a near infrared/pH dual stimuli-responsive activated procedural antibacterial system that combines enhanced antibiotic delivery with photothermal therapy and has highly efficient antimicrobial activity . The antibacterial effect of this therapy was based on two mechanisms of action: chemotherapy, in which the bacterial cell wall was first destroyed, followed by photothermal therapy. After exposure to irradiation with an 808 nm laser, the inhibition rates were 99.8% and 99.1% for Staphylococcus aureus and Pseudomonas aeruginosa , respectively, and the clearance rates for their established biofilms were 75.3% and 74.8%, respectively. Thus, this procedural antibacterial therapy has shown great potentiality for use in the photothermal therapy of bacterial infectious diseases, including biofilm elimination.
研究领域:
微生物学
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纳米医学
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感染性疾病治疗
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Yuan Ma,Bingzhu Wang,Haiwang Wang,Xingyuan Zhao,Yihao Zhao,Songyang Wu,Changxiang Xie
Zinc cadmium sulfide solid solution as a photocatalytic material has the advantages of narrow band gap and suitable conduction band potential, but the fast rate of photogenerated electron-hole recombination is a non-negligible problem. Inspired by the efficient transfer of bioelectric current between neuronal cells, we achieved the modulation of 1% MCNTs-Zn 0.3 Cd 0.7 S microscopic morphology by regulating the ratio of oleic acid and oleylamine during the hydrothermal process, and further constructed the photogenerated carrier transport pathway through the introduction of Pd to improve the rate of hydrogen production from photolytic water. The results showed that the addition of oleic acid and oleylamine resulted in higher crystalline aggregation and smaller peripheral size of the composite materials. The incorporation of both carbon nanotubes and Pd gives the composite's a high photoresponse as well as a low impedance. These are reflected in the photocatalytic hydrogen production rate: the photocatalytic hydrogen production rate of 1% MCNTs-Zn 0.3 Cd 0.7 S/4% Pd reaches 3.889 mmol/g/h, and its photocatalytic rate is 8.89 times higher than that of Zn 0.3 Cd 0.7 S.
研究领域:
材料科学
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光催化
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产品关联
DOI
高影响因子
IN VITRO CELLULAR & DEVELOPMENTAL BIOLOGY-ANIMAL
·
2023
·Vol. 59
·期 3
·193-203
·
IF 2.1
Li Zhe,Jiang Da,Liu Fengling,Li Ying
Palmitoylation is a post-translational modification occurring on cysteine residues, which process is catalyzed by a family of zinc finger Asp-His-His-Cys (DHHC) domain-containing (ZDHHC) protein acyltransferases. As a family member, ZDHHC9 plays a crucial role in varied malignancies by regulating protein stability via protein substrate palmitoylation. Based on the bioinformatic analysis of GEO gene microarray GSE75037 (|log 2 fold change|> 1, P < 0.05), ZDHHC9 was defined as a significantly upregulated gene in lung adenocarcinoma (LUAD), which was also confirmed in our collected clinical specimens. It is necessary to explore the biological function of ZDHHC9 in LUAD cells. The follow-up functional experiments revealed that ZDHHC9 deficiency inhibited proliferation, migration, and invasion, while stimulated apoptosis in HCC827 cells. Besides, these malignant phenotypes could be accelerated by ZDHHC9 overexpression in A549. Moreover, we revealed that ZDHHC9 knockdown could promote PD-L1 protein degradation by reducing its palmitoylation level. The reduction of PD-L1 protein level could enhance anti-tumor immunity and inhibit the growth of LUAD cells. Therefore, our study uncovers the tumor-promoting role of ZDHHC9 in LUAD via regulating PD-L1 stability through palmitoylation, highlighting ZDHHC9 as a novel therapeutic target for LUAD. Graphical abstract
研究领域:
肿瘤学
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分子生物学
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癌症免疫学
✓ 已验证
DOI
PubMed
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Yange Suo,Yuxin Guo,Chenbin Rong,Zhiguo Zhang,Guilin Hu
This work reports the synthesis of a series of carbon supported Pt-Pd-Cu (Pt-Pd-Cu/C) nano-catalysts for formic acid oxidation. The trimetallic catalysts were prepared by a one-pot protocol through reduction of Pt, Pd and Cu ions using ethylene glycol and sodium citrate as the reducing and stabilizing reagents. XRD characterization suggests that Pt-Pd-Cu alloys with different lattice parameters can be successfully prepared through adjusting the atomic ratios of Pt, Pd and Cu ions in the precursor solutions. The average crystal sizes of the Pt-Pd-Cu/C catalysts are in the range of 2.7-3.1 nm. TEM images shows that the metallic nanoparticles are well dispersed on the carbon surface, with Pt 1 Pd 3 Cu 3 /C catalyst showing obvious aggregation. XPS was carried out to analyze the surface compositions, as well as the chemical states of the novel metals in the catalysts. The real atomic ratios of the metals in the catalysts based on ICP-OES evaluation are consistent with the stoichiometric values. Electrochemical analysis suggests that the activities the Pt-Pd-Cu/C catalysts towards formic acid oxidation are dependent on the composition of the catalysts, with Pt 1 Pd 4 Cu 2 /C exhibiting the best performance. A mass normalized peak current density of 3.02 A/mg (Pt+Pd) was observed on Pt 1 Pd 4 Cu 2 /C catalyst.
研究领域:
催化化学
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材料科学
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电化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Fengshun Wu,Li Zeng,Lihua Zhu,Weizhen Wang,Chenghao Cao,Zhiqing Yang,Congxiao Shang,Hengqiang Ye,Zhengxiao Guo
Methanol and ethanol are liquid carriers of hydrogen, convenient and safe to store and transport, particularly of interest as mobile and marine fuels. These can be directly fed into a fuel cell to impart clean energy efficiently, only if their conversion can be cost-effectively catalyzed. In this regard, a cooperative catalyst is developed with atomic Pd species, in the form of single atoms and nanoclusters, dispersed over non-noble bi-metallic CoNi alloy nanoparticles, further supported on reduced graphene oxide (rG) (Pd@CoNi/rG). The catalyst demonstrates a methanol (ethanol) oxidation, MOR (EOR), mass activity (MA) of 1.730 (3.917) A mg −1 Pd (or Pt) , 4.55 (60.26) times greater than that of the commercial 20 wt% Pt/C and 8.65 (20.61) times higher than that of the commercial 20 wt% Pd/C, respectively. More importantly, the catalyst shows excellent stability, maintaining 83.7% (93.7%) of the initial performance after chronoamperometry (CA) for 50000 s in a solution of 1 M KOH + 1 M CH 3 OH (CH 3 CH 2 OH). It significantly out-performs other mono-/bi- metallic counterparts, e.g., Co/rG, Ni/rG, Pd/rG, CoNi/rG, Pd@Co/rG and Pd@Ni/rG, due to its unique cooperative nanostructure with synergistic effects of the different metal (Pd, Co and Ni)-related species.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Dongdong Chen,Huarong Lei,Wuwan Xiong,Ying Li,Xiang Ji,Jia-Yue Yang,Baoxiang Peng,Mingli Fu,Peirong Chen,Daiqi Ye
Phosphorus (P) originating from lubricant oil additives or biofuels is an emerging chemical poison in catalytic systems for automotive exhaust after-treatment. Here, we demonstrate that P-poisoning led to severe deactivation of small-pore Pd-SSZ-13 zeolites (with CHA framework) as passive NOx adsorbers (PNA) and CO oxidation catalysts for cold-start exhaust purification applications. Deactivation mechanisms of P-poisoning were unraveled by comparatively examining the P-free and P-loaded Pd-SSZ-13 zeolites using transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), nuclear magnetic resonance (NMR), temperature-programmed reduction by hydrogen (H2-TPR), CO pulse adsorption, temperature-programmed desorption using NH3 as a probe molecule (NH3-TPD), ultraviolet/visible light (UV/vis) spectroscopy, and in situ diffuse relectance infrared Fourier transform spectroscopy (DRIFTS). The loss of isolated Pd sites─namely, [Pd(OH)]+ and Pd2+ (located in the eight- and six-membered rings of CHA framework, respectively)─was revealed to be largely responsible for the deactivation of Pd-SSZ-13 in passive NOx adsorption and catalytic CO oxidation. In situ DRIFTS studies using NO or CO as a probe molecule suggest that [Pd(OH)]+ was more susceptible to P-poisoning than Pd2+. Specifically, P-poisoning led to a migration of [Pd(OH)]+ from cationic exchange sites to the zeolite surface, forming inactive metaphosphate (i.e., [Pd(OH)]+PO3–) and bulk PdOx species at high temperatures. In contrast, P-poisoning of Pd2+ sites proceeded via a sequential transformation to [Pd(OH)]+ first, and then to [Pd(OH)]+PO3– and bulk PdOx. This study provides a comprehensive mechanistic understanding on the deactivation of Pd-SSZ-13 by P-poisoning, and may guide the design of high-performance, phosphorus-resistant Pd-zeolite catalysts for cold-start exhaust after-treatment.
研究领域:
催化材料
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）