Hydrogen production through hydrogen evolution reaction(HER)offers a promising solution to combat climate change by replacing fossil fuels with clean energy sources.However,the widespread adoption of efficient electro...Hydrogen production through hydrogen evolution reaction(HER)offers a promising solution to combat climate change by replacing fossil fuels with clean energy sources.However,the widespread adoption of efficient electrocatalysts,such as platinum(Pt),has been hindered by their high cost.In this study,we developed an easy-to-implement method to create ultrathin Pt nanomembranes,which catalyze HER at a cost significantly lower than commercial Pt/C and comparable to non-noble metal electrocatalysts.These Pt nanomembranes consist of highly distorted Pt nanocrystals and exhibit a heterogeneous elastic strain field,a characteristic rarely seen in conventional crystals.This unique feature results in significantly higher electrocatalytic efficiency than various forms of Pt electrocatalysts,including Pt/C,Pt foils,and numerous Pt singleatom or single-cluster catalysts.Our research offers a promising approach to develop highly efficient and cost-effective low-dimensional electrocatalysts for sustainable hydrogen production,potentially addressing the challenges posed by the climate crisis.展开更多
Antibody-drug conjugates(ADCs)are a new type of targeting antibodies that conjugate with highly toxic anticancer drugs via chemical linkers to exert high specificity and efficient killing of tumor cells,thereby attrac...Antibody-drug conjugates(ADCs)are a new type of targeting antibodies that conjugate with highly toxic anticancer drugs via chemical linkers to exert high specificity and efficient killing of tumor cells,thereby attracting considerable attention in precise oncology therapy.Cetuximab(Cet)is a typical antibody that offers the benefits of good targeting and safety for individuals with advanced and inoperable cutaneous squamous cell carcinoma(cSCC);however,its anti-tumor activity is limited to a single use.Cisplatin(CisPt)shows good curative effects;however,its adverse effects and non-tumor-targeting ability are major drawbacks.In this study,we designed and developed a new ADC based on a new cytotoxic platinum(IV)prodrug(C8Pt(IV))and Cet.The so-called antibody-platinum(IV)prodrugs conjugates,named Cet-C8Pt(IV),showed excellent tumor targeting in cSCC.Specifically,it accurately delivered C8Pt(IV)into tumor cells to exert the combined anti-tumor effect of Cet and CisPt.Herein,metabolomic analysis showed that Cet-C8Pt(IV)promoted cellular apoptosis and increased DNA damage in cSCC cells by affecting the vitamin B6 metabolic pathway in tumor cells,thereby further enhancing the tumor-killing ability and providing a new strategy for clinical cancer treatment using antibody-platinum(IV)prodrugs conjugates.展开更多
Adsorption kinetics of the interaction between Pt, Pd and Rh(defined here as platinum group elements, PGEs)ions and macromolecular organic compounds(MOCs,>10 kDa), including humic acid, carrageenan and bovine serum...Adsorption kinetics of the interaction between Pt, Pd and Rh(defined here as platinum group elements, PGEs)ions and macromolecular organic compounds(MOCs,>10 kDa), including humic acid, carrageenan and bovine serum albumin, and different cutoff fractions of natural organic matter(>1 kDa and >3 kDa) obtained from seawater using centrifugal ultrafiltration devices were investigated. For a given element, all the adsorption kinetics did not reach equilibrium except the interaction between Pt and >1 kDa cutoff, and between Pd and humic acid.For all the tested MOCs, the adsorption kinetics could be divided into two stages, a rapid adsorption process in the first 8 h and the desorption stage after the first 8 h until the equilibrium. The change trend of partition coefficient(log10Kd) values with experiment time was consistent with that of the kinetic curves. However, in the interaction between PGE ions and natural dissolved organic matter(NDOM), an obvious difference in the change trends of log10Kd and kinetic curves was observed. It indicated that the partition behavior of PGE ions interacting with NDOM in seawater was a combined effect of different organic constituents. The adsorption and log10Kd of PGEs in the >1 kDa NDOM fraction were higher and more stable than those in the >3 kDa NDOM fraction. The results also indicated that the 1–3 kDa NDOM may dominate the interaction between PGEs ions and NDOM. Moreover, no kinetic model could perfectly simulate the adsorption process. It indicated that the colloidal struction and morphology of MOCs or NDOM in seawater might be inhomogeneous. Hence, the interaction between PGE ions and organic matter in seawater was a complicated process and needs further research.展开更多
The kinetics of catalytic hydrogenation of ortho-nitrochlorobenzene to 2,2′-dichloroazoxybenzene on platinum/carbon catalyst is investigated in a slurry reactor with the temperature range of 313-343 K, and orthochlor...The kinetics of catalytic hydrogenation of ortho-nitrochlorobenzene to 2,2′-dichloroazoxybenzene on platinum/carbon catalyst is investigated in a slurry reactor with the temperature range of 313-343 K, and orthochloroaniline is formed as a byproduct. Models based on Rideal-Eley and Langmuir-Hinshelwood mechanism have been proposed based on the rate data and the kinetic regime. The former model can be used to fit the experimental data better. Reaction controlling steps are physical adsorption of hydrogen and adsorbed ortho-nitrochlorobenzene reacted on the surface of catalyst.展开更多
A highly sensitive double artificial neural network (DANN) analysis with flow-injection chemiluminescence (FI-CL) has been developed to simultaneously determine the trace amounts of the gold and platinum in simula...A highly sensitive double artificial neural network (DANN) analysis with flow-injection chemiluminescence (FI-CL) has been developed to simultaneously determine the trace amounts of the gold and platinum in simulated mixed samples, without the boring process.展开更多
Network crewn ether polymer with pendant sulfide side ohain in the networkstructure units has been synthesized via ring- opening copolymerization of β-ethylthioethyl glycidyl ether and diethylene glycol bisglycidyl e...Network crewn ether polymer with pendant sulfide side ohain in the networkstructure units has been synthesized via ring- opening copolymerization of β-ethylthioethyl glycidyl ether and diethylene glycol bisglycidyl ether. A kind of active catalyst suitable for this reaction was suggested. The title polymer was found tobe a good ligand for platinous chloride, and the platinous complex could catalyze thehydrosilylation of olefins with triethoxysilane efficiently.展开更多
Objective:The choice of chemotherapeutic regimen for triple-negative breast cancer(TNBC)remains controversial.Homologous recombination deficiency(HRD)has attracted increasing attention in informing chemotherapy treatm...Objective:The choice of chemotherapeutic regimen for triple-negative breast cancer(TNBC)remains controversial.Homologous recombination deficiency(HRD)has attracted increasing attention in informing chemotherapy treatment.This study was aimed at investigating the feasibility of HRD as a clinically actionable biomarker for platinum-containing and platinum-free therapy.Methods:Chinese patients with TNBC who received chemotherapy between May 1,2008 and March 31,2020 were retrospectively analyzed with a customized 3D-HRD panel.HRD positivity was defined by an HRD score≥30 or deleterious BRCA1/2 mutation.A total of 386 chemotherapy-treated patients with TNBC were screened from a surgical cohort(NCT01150513)and a metastatic cohort,and 189 patients with available clinical and tumor sequencing data were included.Results:In the entire cohort,49.2%(93/189)of patients were identified as HRD positive(40 with deleterious BRCA1/2 mutations and 53 with BRCA1/2 intact with an HRD score of≥30).In the first-line metastatic setting,platinum therapy was associated with longer median progression-free survival(mPFS)than platinum-free therapy[9.1 vs.3.0 months;hazard ratio(HR),0.43;95%confidence interval 0.22–0.84;P=0.01].Among HRD-positive patients,the mPFS was significantly longer in those treated with platinum rather than platinum-free therapy(13.6 vs.2.0 months;HR,0.11;P=0.001).Among patients administered a platinum-free regimen,HRD-negative patients showed a PFS significantly superior to that of HRD-positive patients(P=0.02;treatment-biomarker P-interaction=0.001).Similar results were observed in the BRCA1/2-intact subset.In the adjuvant setting,HRD-positive patients tended to benefit more from platinum chemotherapy than from platinum-free chemotherapy(P=0.05,P-interaction=0.02).Conclusions:HRD characterization may guide decision-making regarding the use of platinum treatment in patients with TNBC in both adjuvant and metastatic settings.展开更多
The title polymer was prepared from 5-diethylamino-3-thia-pentyl glycidyl ether anddiethylene glycol bisglycidyl ether via ring-opening copolymerization. It was found that thisreaction could be catalyzed by sodium, bu...The title polymer was prepared from 5-diethylamino-3-thia-pentyl glycidyl ether anddiethylene glycol bisglycidyl ether via ring-opening copolymerization. It was found that thisreaction could be catalyzed by sodium, but not Lewis acid. The obtained polymer can coordinatewith platinum compound, and the platinum complex is a new kind of catalyst for thehydrosilylation of olefins with triethoxysilane.展开更多
Studies were performed in 20 patients with breast cancer, who received 26 cycles of high-dose cisplatin (100 mg/m2, IV. drip). In twenty-five cycles of them urinary Alb, IgG and NAG showed abnormal values. The patient...Studies were performed in 20 patients with breast cancer, who received 26 cycles of high-dose cisplatin (100 mg/m2, IV. drip). In twenty-five cycles of them urinary Alb, IgG and NAG showed abnormal values. The patients were divided into low-nephrotoxicity and high-nephrotoxicity groups by the degree of renal dysfunction. Thirty-five percent of the patients exhibited high-nephrotoxicity. These patients had significantly higher plasma and/ or urinary Pt peak levels during cisplatin (CP) infusion than did low-nephrotoxicity. 70 - 80% of the patients developed significant nephrotoxicity when urinary Pt peak level rose up to 40 fig/ml or plasma Pt peak level >4 μg/ml. It is quite important to reduce nephrotoxicity that urinary Pt level is controlled below 40 μg/ml and plasma Pt level <4 μg/ml. It is suggested that urine output should be maintained over 300 ml/hr during 2 hours before and after the end of infusion and >100 ml/hr during 3 days after the infusion. That may keep the nephrotoxicity of CP in less serious degree and easy to recover.展开更多
Background:Despite immunotherapy advancements for patients with advanced or metastatic non-small-cell lung cancer(NSCLC),pivotal first-line trials were limited to patients with an Eastern Cooperative Oncology Group pe...Background:Despite immunotherapy advancements for patients with advanced or metastatic non-small-cell lung cancer(NSCLC),pivotal first-line trials were limited to patients with an Eastern Cooperative Oncology Group performance status(ECOG PS)0-1 and a median age of 65 years or younger.We aimed to compare the efficacy and safety of first-line atezolizumab monotherapy with single-agent chemotherapy in patients ineligible for platinum-based chemotherapy.Methods:This trial was a phase 3,open-label,randomised controlled study conducted at 91 sites in 23 countries across Asia,Europe,North America,and South America.Eligible patients had stage IIIB or IV NSCLC in whom platinum-doublet chemotherapy was deemed unsuitable by the investigator due to an ECOG PS 2 or 3,or alternatively,being 70 years or older with an ECOG PS 0-1 with substantial comorbidities or contraindications for platinum-doublet chemotherapy.Patients were randomised 2:1 by permuted-block randomisation(block size of six)to receive 1200 mg of atezolizumab given intravenously every 3 weeks or single-agent chemotherapy(vinorelbine[oral or intravenous]or gemcitabine[intravenous];dosing per local label)at 3-weekly or 4-weekly cycles.The primary endpoint was overall survival assessed in the intention-to-treat population.Safety analyses were conducted in the safety-evaluable population,which included all randomised patients who received any amount of atezolizumab or chemotherapy.This trial is registered with ClinicalTrials.gov,NCT03191786.展开更多
The shuttle effect derived from diffusion of lithium polysulfides(LiPSs) and sluggish redox kinetic bring about poor cycling stability and low utilization of sulfur,which have always been the key challenging issues fo...The shuttle effect derived from diffusion of lithium polysulfides(LiPSs) and sluggish redox kinetic bring about poor cycling stability and low utilization of sulfur,which have always been the key challenging issues for the commercial application of lithium-sulfur(Li-S) batteries.Rational design of cathode materials to catalyze Li_(2)S dissociation/nucleation processes is an appealing and valid strategy to develop high-energy practical Li-S batteries.Herein,considering the synergistic effect of bidirectional catalysis on LiPSs conversion and enhanced chemical immobilization for LiPSs by heteroatom doping,Pt nanoparticles loaded on nitrogen-doped carbon spheres(Pt/NCS composites) were constructed as cathode materials.According to the dynamic evolution of Pt catalysts and sulfur species,Pt~0 and Pt^(2+) species were identified as active species for the accelerated dissociation and nucleation of Li_(2)S,respectively.Meanwhile,in-situ Raman results demonstrated the expedited conversion of sulfur species resulted from bidirectional catalysis of active Pt species,corresponding to boosted redox kinetics.Consequently,Pt/NCS cathode exhibited improved long-term cyclability with high initial capacity,along with enhanced rate capability.This work provides a facile approach to construct cathode materials with bidirectional catalysis on Li_(2)S dissociation/nucleation,and sheds light on a more global understanding of the catalytic mechanism of metal catalysts during LiPSs conversion.展开更多
Both structure and interface engineering are highly effective strategies for enhancing the catalytic activity and selectivity of precious metal nanostructures.In this work,we develop a facile pyrolysis strategy to syn...Both structure and interface engineering are highly effective strategies for enhancing the catalytic activity and selectivity of precious metal nanostructures.In this work,we develop a facile pyrolysis strategy to synthesize the high-quality holey platinum nanotubes(Pt-H-NTs)using nanorods-like Pt^(Ⅱ)-phenanthroline(PT)coordination compound as self-template and self-reduction precursor.Then,an up-bottom strategy is used to further synthesize polyallylamine(PA)modified Pt-H-NTs(Pt-HNTs@PA).PA modification sharply promotes the catalytic activity of Pt-H-NTs for the formic acid electrooxidation reaction(FAEOR)by the direct reaction pathway.Meanwhile,PA modification also elevates the catalytic activity of Pt-H-NTs for the hydrogen evolution reaction(HER)by the proton enrichment at electrolyte/electrode interface.Benefiting from the high catalytic activity of Pt-H-NTs@PA for both FAEOR and HER,a two-electrode FAEOR boosted water electrolysis system is fabricated by using Pt-H-NTs@PA as bifunctio nal electrocatalysts.Such FAEOR boosted water electrolysis system only requires the operational voltage of 0.47 V to achieve the high-purity hydrogen production,showing an energy-saving hydrogen production strategy compared to traditional water electrolysis system.展开更多
A three-dimensional graphene-based composite was prepared by a simple one-step in-site reduced-oxide method under atmospheric pressure. The obtained hydrogel was modified with 4-amino-benzenesulfonic acid and connecte...A three-dimensional graphene-based composite was prepared by a simple one-step in-site reduced-oxide method under atmospheric pressure. The obtained hydrogel was modified with 4-amino-benzenesulfonic acid and connected with ethylenediamine, and freeze-dried into an aerogel, which was characterized. Then the surface interaction with platinum (Pt, IV) was explored. The obtained aerogel showed good adsorption for Pt (IV) at acid conditions, giving a rising to the adsorption rate > 98% while pH ≥ 6. Using hexadecyl trimethyl ammonium bromide of 2% (m/V) as an eluent to desorb the Pt (IV) from the surface of the aerogel, a desorption rate of 81.1% was obtained in this process. Urea, buffer aquation and other surfactants were used in the desorption experiment to understand the adsorption mechanism between the aerogel and Pt (IV). In this work, hydrogen bond, van der Waals force and electronic interaction force mainly drove the adsorption process. For obtaining more purified Pt (IV), we used 0.5% CTAB to desorb Pd (II). A new three-dimensional graphene-based composite was prepared and the surface interaction between Pt (IV) and composite was experimented for understanding the adsorption mechanism and exploring its potential application in sample preparation in low concentration.展开更多
Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reactio...Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reaction(HOR).Herein,we describe the synthesis of a Pt single electrocatalyst inside single-walled carbon nanotubes(SWCNTs)via a redox reaction.Characterizations via electron microscopy,X-ray photoelectron microscopy,and X-ray absorption spectroscopy show the single-atom nature of the Pt.The electrochemical behavior of the sample to hydrogen and oxygen was investigated using the advanced floating electrode technique,which minimizes mass transport limitations and gives a thorough insight into the activity of the electrocatalyst.The single-atom samples showed higher HOR activity than state-of-the-art 30%Pt/C while almost no oxygen reduction reaction activity in the proton exchange membrane fuel cell operating range.The selective activity toward HOR arose as the main fingerprint of the catalyst confinement in the SWCNTs.展开更多
The scarcity,high cost and susceptibility to CO of Platinum severely restrict its application in alkaline hydrogen oxidation reaction(HOR).Hybridizing Pt with other transition metals provides an effective strategy to ...The scarcity,high cost and susceptibility to CO of Platinum severely restrict its application in alkaline hydrogen oxidation reaction(HOR).Hybridizing Pt with other transition metals provides an effective strategy to modulate its catalytic HOR performance,but at the cost of mass activity due to the coverage of modifiers on Pt surface.Herein,we constructed dual junctions'Pt/nitrogen-doped carbon(Pt/NC)andδ-MoC/NC to modify electronic structure of Pt via interfacial electron transfer to acquire Pt-MoC@NC catalyst with electron-deficient Pt nanoparticles,simultaneously endowing it with high mass activity and durability of alkaline HOR.Moreover,the unique structure of Pt-MoC@NC endows Pt with a high COtolerance at 1,000 ppm CO/H_(2),a quality that commercial Pt-C catalyst lacks.The theoretical calculations not only confirm the diffusion of electrons from Pt/NC to Mo C/NC could occur,but also demonstrate the negative shift of Pt d-band center for the optimized binding energies of*H,*OH and CO.展开更多
A new lifetime control technique-localized platinum lifetime control (LPLC) is introduced. Silicon samples are implanted with 550keV protons at dosages from 1 × 10^13 to 5 × 10^14 cm^-2. Subsequently, plat...A new lifetime control technique-localized platinum lifetime control (LPLC) is introduced. Silicon samples are implanted with 550keV protons at dosages from 1 × 10^13 to 5 × 10^14 cm^-2. Subsequently, platinum diffusion in silicon is performed at 700 or 750℃ for 15 or 30min,respectively. Then the in-diffused platinum into damaged regions of the proton-implanted silicon is investigated by use of deep-level transient spectroscopy (DLTS). Finally, for all of the LPLC samples, the distribution of the in-diffused substitutional platinum agrees well with the damage distribution resulting from the low-dosage proton implantation. Also, the diodes show a very low leakage current even at elevated temperatures while keeping the major advantages of ion irradiation devices, including low turn-off loss and soft recovery.展开更多
Flare and multiple recurrences pose significant challenges in gouty arthritis.Traditional treatments provide temporary relief from inflammation but fail to promptly alleviate patient pain or effectively prevent subseq...Flare and multiple recurrences pose significant challenges in gouty arthritis.Traditional treatments provide temporary relief from inflammation but fail to promptly alleviate patient pain or effectively prevent subsequent recurrences.It should also be noted that both anti-inflammation and metabolism of uric acid are necessary for gouty arthritis,calling for therapeutic systems to achieve these two goals simultaneously.In this study,we propose a biomimetic integrated nanozyme,HMPB-Pt@MM,comprising platinum nanozyme and hollow Prussian blue.It demonstrates anti-inflammatory properties by eliminating reactive oxygen species and reducing infiltration of inflammatory macrophages.Additionally,it rapidly targets inflamed ankles through the camouflage of macrophage membranes.Furthermore,HMPB-Pt@MM exhibits urate oxidase-like capabilities,continuously metabolizing locally elevated uric acid concentrations,ultimately inhibiting multiple recurrences of gouty arthritis.In summary,HMPB-Pt@MM integrates ROS clearance with uric acid metabolism,offering a promising platform for the treatment of gouty arthritis.展开更多
Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this s...Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ synthesis.These~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt ions.This unique structure is beneficial for the hydrogen evolution reaction.The catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C catalysts.Mass activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.展开更多
The long-range periodically ordered atomic structures in intermetallic nanoparticles(INPs)can significantly enhance both the electrocatalytic activity and electrochemical stability toward the oxygen reduction reaction...The long-range periodically ordered atomic structures in intermetallic nanoparticles(INPs)can significantly enhance both the electrocatalytic activity and electrochemical stability toward the oxygen reduction reaction(ORR)compared to the disordered atomic structures in ordinary solid-solution alloy NPs.Accordingly,through a facile and scalable synthetic method,a series of carbon-supported ultrafine Pt_3Co_(x)Mn_(1-x)ternary INPs are prepared in this work,which possess the"skin-like"ultrathin Pt shells,the ordered L1_(2) atomic structure,and the high-even dispersion on supports(L1_(2)-Pt_3Co_(x)Mn_(1-x)/~SPt INPs/C).Electrochemical results present that the composition-optimized L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C exhibits the highest electrocata lytic activity among the series,which are also much better than those of the pristine ultrafine Pt/C.Besides,it also has a greatly enhanced electrochemical stability.In addition,the effects of annealing temperature and time are further investigated.More importantly,such superior ORR electrocatalytic performance of L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C are also well demonstrated in practical fuel cells.Physicochemical characterization analyses further reveal the major origins of the greatly enhanced ORR electrocata lytic performance:the Pt-Co-Mn alloy-induced geometric and ligand effects as well as the extremely high L1_(2) atomic-ordering degree.This work not only successfully develops a highly active and stable ordered ternary intermetallic ORR electrocatalyst,but also elucidates the corresponding"structure-function"relationship,which can be further applied in designing other intermetallic(electro)catalysts.展开更多
基金The research of YY is supported by the Research Grant Council(RGC)through the General Research Fund(GRF)with the grant number N_CityU 109/21,CityU11213118 and CityU11209317.
文摘Hydrogen production through hydrogen evolution reaction(HER)offers a promising solution to combat climate change by replacing fossil fuels with clean energy sources.However,the widespread adoption of efficient electrocatalysts,such as platinum(Pt),has been hindered by their high cost.In this study,we developed an easy-to-implement method to create ultrathin Pt nanomembranes,which catalyze HER at a cost significantly lower than commercial Pt/C and comparable to non-noble metal electrocatalysts.These Pt nanomembranes consist of highly distorted Pt nanocrystals and exhibit a heterogeneous elastic strain field,a characteristic rarely seen in conventional crystals.This unique feature results in significantly higher electrocatalytic efficiency than various forms of Pt electrocatalysts,including Pt/C,Pt foils,and numerous Pt singleatom or single-cluster catalysts.Our research offers a promising approach to develop highly efficient and cost-effective low-dimensional electrocatalysts for sustainable hydrogen production,potentially addressing the challenges posed by the climate crisis.
基金the National Natural Science Foundation of China(Grant No.:51803120).
文摘Antibody-drug conjugates(ADCs)are a new type of targeting antibodies that conjugate with highly toxic anticancer drugs via chemical linkers to exert high specificity and efficient killing of tumor cells,thereby attracting considerable attention in precise oncology therapy.Cetuximab(Cet)is a typical antibody that offers the benefits of good targeting and safety for individuals with advanced and inoperable cutaneous squamous cell carcinoma(cSCC);however,its anti-tumor activity is limited to a single use.Cisplatin(CisPt)shows good curative effects;however,its adverse effects and non-tumor-targeting ability are major drawbacks.In this study,we designed and developed a new ADC based on a new cytotoxic platinum(IV)prodrug(C8Pt(IV))and Cet.The so-called antibody-platinum(IV)prodrugs conjugates,named Cet-C8Pt(IV),showed excellent tumor targeting in cSCC.Specifically,it accurately delivered C8Pt(IV)into tumor cells to exert the combined anti-tumor effect of Cet and CisPt.Herein,metabolomic analysis showed that Cet-C8Pt(IV)promoted cellular apoptosis and increased DNA damage in cSCC cells by affecting the vitamin B6 metabolic pathway in tumor cells,thereby further enhancing the tumor-killing ability and providing a new strategy for clinical cancer treatment using antibody-platinum(IV)prodrugs conjugates.
基金The National Natural Science Foundation of China under contract No.41376083the Strategic Priority Research Program of the Chinese Academy of Sciences under contract No.XDA23050303
文摘Adsorption kinetics of the interaction between Pt, Pd and Rh(defined here as platinum group elements, PGEs)ions and macromolecular organic compounds(MOCs,>10 kDa), including humic acid, carrageenan and bovine serum albumin, and different cutoff fractions of natural organic matter(>1 kDa and >3 kDa) obtained from seawater using centrifugal ultrafiltration devices were investigated. For a given element, all the adsorption kinetics did not reach equilibrium except the interaction between Pt and >1 kDa cutoff, and between Pd and humic acid.For all the tested MOCs, the adsorption kinetics could be divided into two stages, a rapid adsorption process in the first 8 h and the desorption stage after the first 8 h until the equilibrium. The change trend of partition coefficient(log10Kd) values with experiment time was consistent with that of the kinetic curves. However, in the interaction between PGE ions and natural dissolved organic matter(NDOM), an obvious difference in the change trends of log10Kd and kinetic curves was observed. It indicated that the partition behavior of PGE ions interacting with NDOM in seawater was a combined effect of different organic constituents. The adsorption and log10Kd of PGEs in the >1 kDa NDOM fraction were higher and more stable than those in the >3 kDa NDOM fraction. The results also indicated that the 1–3 kDa NDOM may dominate the interaction between PGEs ions and NDOM. Moreover, no kinetic model could perfectly simulate the adsorption process. It indicated that the colloidal struction and morphology of MOCs or NDOM in seawater might be inhomogeneous. Hence, the interaction between PGE ions and organic matter in seawater was a complicated process and needs further research.
文摘The kinetics of catalytic hydrogenation of ortho-nitrochlorobenzene to 2,2′-dichloroazoxybenzene on platinum/carbon catalyst is investigated in a slurry reactor with the temperature range of 313-343 K, and orthochloroaniline is formed as a byproduct. Models based on Rideal-Eley and Langmuir-Hinshelwood mechanism have been proposed based on the rate data and the kinetic regime. The former model can be used to fit the experimental data better. Reaction controlling steps are physical adsorption of hydrogen and adsorbed ortho-nitrochlorobenzene reacted on the surface of catalyst.
文摘A highly sensitive double artificial neural network (DANN) analysis with flow-injection chemiluminescence (FI-CL) has been developed to simultaneously determine the trace amounts of the gold and platinum in simulated mixed samples, without the boring process.
文摘Network crewn ether polymer with pendant sulfide side ohain in the networkstructure units has been synthesized via ring- opening copolymerization of β-ethylthioethyl glycidyl ether and diethylene glycol bisglycidyl ether. A kind of active catalyst suitable for this reaction was suggested. The title polymer was found tobe a good ligand for platinous chloride, and the platinous complex could catalyze thehydrosilylation of olefins with triethoxysilane efficiently.
基金granted by Capital’s Funds for Health Improvement and Research(Grant No.2018-2-4023)the National Natural Science Foundation of China(Grant No.82001559)。
文摘Objective:The choice of chemotherapeutic regimen for triple-negative breast cancer(TNBC)remains controversial.Homologous recombination deficiency(HRD)has attracted increasing attention in informing chemotherapy treatment.This study was aimed at investigating the feasibility of HRD as a clinically actionable biomarker for platinum-containing and platinum-free therapy.Methods:Chinese patients with TNBC who received chemotherapy between May 1,2008 and March 31,2020 were retrospectively analyzed with a customized 3D-HRD panel.HRD positivity was defined by an HRD score≥30 or deleterious BRCA1/2 mutation.A total of 386 chemotherapy-treated patients with TNBC were screened from a surgical cohort(NCT01150513)and a metastatic cohort,and 189 patients with available clinical and tumor sequencing data were included.Results:In the entire cohort,49.2%(93/189)of patients were identified as HRD positive(40 with deleterious BRCA1/2 mutations and 53 with BRCA1/2 intact with an HRD score of≥30).In the first-line metastatic setting,platinum therapy was associated with longer median progression-free survival(mPFS)than platinum-free therapy[9.1 vs.3.0 months;hazard ratio(HR),0.43;95%confidence interval 0.22–0.84;P=0.01].Among HRD-positive patients,the mPFS was significantly longer in those treated with platinum rather than platinum-free therapy(13.6 vs.2.0 months;HR,0.11;P=0.001).Among patients administered a platinum-free regimen,HRD-negative patients showed a PFS significantly superior to that of HRD-positive patients(P=0.02;treatment-biomarker P-interaction=0.001).Similar results were observed in the BRCA1/2-intact subset.In the adjuvant setting,HRD-positive patients tended to benefit more from platinum chemotherapy than from platinum-free chemotherapy(P=0.05,P-interaction=0.02).Conclusions:HRD characterization may guide decision-making regarding the use of platinum treatment in patients with TNBC in both adjuvant and metastatic settings.
基金This work was supported by the National Natural Science Foundation of China
文摘The title polymer was prepared from 5-diethylamino-3-thia-pentyl glycidyl ether anddiethylene glycol bisglycidyl ether via ring-opening copolymerization. It was found that thisreaction could be catalyzed by sodium, but not Lewis acid. The obtained polymer can coordinatewith platinum compound, and the platinum complex is a new kind of catalyst for thehydrosilylation of olefins with triethoxysilane.
文摘Studies were performed in 20 patients with breast cancer, who received 26 cycles of high-dose cisplatin (100 mg/m2, IV. drip). In twenty-five cycles of them urinary Alb, IgG and NAG showed abnormal values. The patients were divided into low-nephrotoxicity and high-nephrotoxicity groups by the degree of renal dysfunction. Thirty-five percent of the patients exhibited high-nephrotoxicity. These patients had significantly higher plasma and/ or urinary Pt peak levels during cisplatin (CP) infusion than did low-nephrotoxicity. 70 - 80% of the patients developed significant nephrotoxicity when urinary Pt peak level rose up to 40 fig/ml or plasma Pt peak level >4 μg/ml. It is quite important to reduce nephrotoxicity that urinary Pt level is controlled below 40 μg/ml and plasma Pt level <4 μg/ml. It is suggested that urine output should be maintained over 300 ml/hr during 2 hours before and after the end of infusion and >100 ml/hr during 3 days after the infusion. That may keep the nephrotoxicity of CP in less serious degree and easy to recover.
文摘Background:Despite immunotherapy advancements for patients with advanced or metastatic non-small-cell lung cancer(NSCLC),pivotal first-line trials were limited to patients with an Eastern Cooperative Oncology Group performance status(ECOG PS)0-1 and a median age of 65 years or younger.We aimed to compare the efficacy and safety of first-line atezolizumab monotherapy with single-agent chemotherapy in patients ineligible for platinum-based chemotherapy.Methods:This trial was a phase 3,open-label,randomised controlled study conducted at 91 sites in 23 countries across Asia,Europe,North America,and South America.Eligible patients had stage IIIB or IV NSCLC in whom platinum-doublet chemotherapy was deemed unsuitable by the investigator due to an ECOG PS 2 or 3,or alternatively,being 70 years or older with an ECOG PS 0-1 with substantial comorbidities or contraindications for platinum-doublet chemotherapy.Patients were randomised 2:1 by permuted-block randomisation(block size of six)to receive 1200 mg of atezolizumab given intravenously every 3 weeks or single-agent chemotherapy(vinorelbine[oral or intravenous]or gemcitabine[intravenous];dosing per local label)at 3-weekly or 4-weekly cycles.The primary endpoint was overall survival assessed in the intention-to-treat population.Safety analyses were conducted in the safety-evaluable population,which included all randomised patients who received any amount of atezolizumab or chemotherapy.This trial is registered with ClinicalTrials.gov,NCT03191786.
基金the financial support provided by the National Natural Science Foundation of China (51932005, 22072164)the Liaoning Revitalization Talents Program (XLYC1807175)+3 种基金the Research Fund of Shenyang National Laboratory for Materials Sciencethe IMR Innovation Fund (2023PY10)the Natural Science Foundation of Liaoning Province (2023-BS-013)the Science and Technology Research Project of Education Department of Jilin Province (JJKH20210453KJ)。
文摘The shuttle effect derived from diffusion of lithium polysulfides(LiPSs) and sluggish redox kinetic bring about poor cycling stability and low utilization of sulfur,which have always been the key challenging issues for the commercial application of lithium-sulfur(Li-S) batteries.Rational design of cathode materials to catalyze Li_(2)S dissociation/nucleation processes is an appealing and valid strategy to develop high-energy practical Li-S batteries.Herein,considering the synergistic effect of bidirectional catalysis on LiPSs conversion and enhanced chemical immobilization for LiPSs by heteroatom doping,Pt nanoparticles loaded on nitrogen-doped carbon spheres(Pt/NCS composites) were constructed as cathode materials.According to the dynamic evolution of Pt catalysts and sulfur species,Pt~0 and Pt^(2+) species were identified as active species for the accelerated dissociation and nucleation of Li_(2)S,respectively.Meanwhile,in-situ Raman results demonstrated the expedited conversion of sulfur species resulted from bidirectional catalysis of active Pt species,corresponding to boosted redox kinetics.Consequently,Pt/NCS cathode exhibited improved long-term cyclability with high initial capacity,along with enhanced rate capability.This work provides a facile approach to construct cathode materials with bidirectional catalysis on Li_(2)S dissociation/nucleation,and sheds light on a more global understanding of the catalytic mechanism of metal catalysts during LiPSs conversion.
基金sponsored by the National Natural Science Foundation of China(22272103)the Natural Science Foundation of Shaanxi Province(2020JZ-23,2019KJXX-021,and 2020JM269)+7 种基金the Key Research and Development Program of Shaanxi(2020SF-355)the Science and Technology Innovation Team of Shaanxi Province(2022TD-35)the University Engineering Research Center of Crystal Growth and Applications of Guangdong Province(2020GCZX005)the Special Innovative Projects of Guangdong Province(2020KTSCX125)the Shenzhen Stable Supporting Program(SZWD2021015)the Fundamental Research Funds for the Central Universities(GK202202001)the Open Foundation of Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials at Guangxi University(2021GXYSOF02)the 111 Project(B14041)。
文摘Both structure and interface engineering are highly effective strategies for enhancing the catalytic activity and selectivity of precious metal nanostructures.In this work,we develop a facile pyrolysis strategy to synthesize the high-quality holey platinum nanotubes(Pt-H-NTs)using nanorods-like Pt^(Ⅱ)-phenanthroline(PT)coordination compound as self-template and self-reduction precursor.Then,an up-bottom strategy is used to further synthesize polyallylamine(PA)modified Pt-H-NTs(Pt-HNTs@PA).PA modification sharply promotes the catalytic activity of Pt-H-NTs for the formic acid electrooxidation reaction(FAEOR)by the direct reaction pathway.Meanwhile,PA modification also elevates the catalytic activity of Pt-H-NTs for the hydrogen evolution reaction(HER)by the proton enrichment at electrolyte/electrode interface.Benefiting from the high catalytic activity of Pt-H-NTs@PA for both FAEOR and HER,a two-electrode FAEOR boosted water electrolysis system is fabricated by using Pt-H-NTs@PA as bifunctio nal electrocatalysts.Such FAEOR boosted water electrolysis system only requires the operational voltage of 0.47 V to achieve the high-purity hydrogen production,showing an energy-saving hydrogen production strategy compared to traditional water electrolysis system.
文摘A three-dimensional graphene-based composite was prepared by a simple one-step in-site reduced-oxide method under atmospheric pressure. The obtained hydrogel was modified with 4-amino-benzenesulfonic acid and connected with ethylenediamine, and freeze-dried into an aerogel, which was characterized. Then the surface interaction with platinum (Pt, IV) was explored. The obtained aerogel showed good adsorption for Pt (IV) at acid conditions, giving a rising to the adsorption rate > 98% while pH ≥ 6. Using hexadecyl trimethyl ammonium bromide of 2% (m/V) as an eluent to desorb the Pt (IV) from the surface of the aerogel, a desorption rate of 81.1% was obtained in this process. Urea, buffer aquation and other surfactants were used in the desorption experiment to understand the adsorption mechanism between the aerogel and Pt (IV). In this work, hydrogen bond, van der Waals force and electronic interaction force mainly drove the adsorption process. For obtaining more purified Pt (IV), we used 0.5% CTAB to desorb Pd (II). A new three-dimensional graphene-based composite was prepared and the surface interaction between Pt (IV) and composite was experimented for understanding the adsorption mechanism and exploring its potential application in sample preparation in low concentration.
基金support from Horizon 2020 program within the ITN FlowcampDZ acknowledges funding from the Wohl Foundation for research for the promotion of UK-Israel research cooperationDZ acknowledges funding from Israel Ministry of Energy(grant#220-11-047).
文摘Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reaction(HOR).Herein,we describe the synthesis of a Pt single electrocatalyst inside single-walled carbon nanotubes(SWCNTs)via a redox reaction.Characterizations via electron microscopy,X-ray photoelectron microscopy,and X-ray absorption spectroscopy show the single-atom nature of the Pt.The electrochemical behavior of the sample to hydrogen and oxygen was investigated using the advanced floating electrode technique,which minimizes mass transport limitations and gives a thorough insight into the activity of the electrocatalyst.The single-atom samples showed higher HOR activity than state-of-the-art 30%Pt/C while almost no oxygen reduction reaction activity in the proton exchange membrane fuel cell operating range.The selective activity toward HOR arose as the main fingerprint of the catalyst confinement in the SWCNTs.
基金supported by the National Natural Science Foundation of China (Grant Nos.52072272,52171145 and 22109120)the Zhejiang Provincial Natural Science Foundation of China (LQ21B030002)+1 种基金the Zhejiang Provincial Special Support Program for High-level Talents (2019R52042)the Key programs for Science and Technology Innovation of Wenzhou (ZG2022037)。
文摘The scarcity,high cost and susceptibility to CO of Platinum severely restrict its application in alkaline hydrogen oxidation reaction(HOR).Hybridizing Pt with other transition metals provides an effective strategy to modulate its catalytic HOR performance,but at the cost of mass activity due to the coverage of modifiers on Pt surface.Herein,we constructed dual junctions'Pt/nitrogen-doped carbon(Pt/NC)andδ-MoC/NC to modify electronic structure of Pt via interfacial electron transfer to acquire Pt-MoC@NC catalyst with electron-deficient Pt nanoparticles,simultaneously endowing it with high mass activity and durability of alkaline HOR.Moreover,the unique structure of Pt-MoC@NC endows Pt with a high COtolerance at 1,000 ppm CO/H_(2),a quality that commercial Pt-C catalyst lacks.The theoretical calculations not only confirm the diffusion of electrons from Pt/NC to Mo C/NC could occur,but also demonstrate the negative shift of Pt d-band center for the optimized binding energies of*H,*OH and CO.
文摘A new lifetime control technique-localized platinum lifetime control (LPLC) is introduced. Silicon samples are implanted with 550keV protons at dosages from 1 × 10^13 to 5 × 10^14 cm^-2. Subsequently, platinum diffusion in silicon is performed at 700 or 750℃ for 15 or 30min,respectively. Then the in-diffused platinum into damaged regions of the proton-implanted silicon is investigated by use of deep-level transient spectroscopy (DLTS). Finally, for all of the LPLC samples, the distribution of the in-diffused substitutional platinum agrees well with the damage distribution resulting from the low-dosage proton implantation. Also, the diodes show a very low leakage current even at elevated temperatures while keeping the major advantages of ion irradiation devices, including low turn-off loss and soft recovery.
基金supported by the National Key R&D Program of the Ministry of Science and Technology (2022YFC2304303)。
文摘Flare and multiple recurrences pose significant challenges in gouty arthritis.Traditional treatments provide temporary relief from inflammation but fail to promptly alleviate patient pain or effectively prevent subsequent recurrences.It should also be noted that both anti-inflammation and metabolism of uric acid are necessary for gouty arthritis,calling for therapeutic systems to achieve these two goals simultaneously.In this study,we propose a biomimetic integrated nanozyme,HMPB-Pt@MM,comprising platinum nanozyme and hollow Prussian blue.It demonstrates anti-inflammatory properties by eliminating reactive oxygen species and reducing infiltration of inflammatory macrophages.Additionally,it rapidly targets inflamed ankles through the camouflage of macrophage membranes.Furthermore,HMPB-Pt@MM exhibits urate oxidase-like capabilities,continuously metabolizing locally elevated uric acid concentrations,ultimately inhibiting multiple recurrences of gouty arthritis.In summary,HMPB-Pt@MM integrates ROS clearance with uric acid metabolism,offering a promising platform for the treatment of gouty arthritis.
基金financially supported by the National Natural Science Foundation of China(No.5217042069)the Young Elite Scientist Sponsorship Program by China Association for Science and Technology(CAST)(No.YESS20200103)the Fundamental Research Funds for the Central Universities(No.265QZ2022004)。
文摘Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ synthesis.These~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt ions.This unique structure is beneficial for the hydrogen evolution reaction.The catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C catalysts.Mass activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.
基金supported by the National Key Research and Development Program of China(2021YFB4001301)the Science and Technology Commission of Shanghai Municipality(21DZ1208600)the Oceanic Interdisciplinary Program of Shanghai Jiao Tong University(SL2021ZD105)。
文摘The long-range periodically ordered atomic structures in intermetallic nanoparticles(INPs)can significantly enhance both the electrocatalytic activity and electrochemical stability toward the oxygen reduction reaction(ORR)compared to the disordered atomic structures in ordinary solid-solution alloy NPs.Accordingly,through a facile and scalable synthetic method,a series of carbon-supported ultrafine Pt_3Co_(x)Mn_(1-x)ternary INPs are prepared in this work,which possess the"skin-like"ultrathin Pt shells,the ordered L1_(2) atomic structure,and the high-even dispersion on supports(L1_(2)-Pt_3Co_(x)Mn_(1-x)/~SPt INPs/C).Electrochemical results present that the composition-optimized L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C exhibits the highest electrocata lytic activity among the series,which are also much better than those of the pristine ultrafine Pt/C.Besides,it also has a greatly enhanced electrochemical stability.In addition,the effects of annealing temperature and time are further investigated.More importantly,such superior ORR electrocatalytic performance of L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C are also well demonstrated in practical fuel cells.Physicochemical characterization analyses further reveal the major origins of the greatly enhanced ORR electrocata lytic performance:the Pt-Co-Mn alloy-induced geometric and ligand effects as well as the extremely high L1_(2) atomic-ordering degree.This work not only successfully develops a highly active and stable ordered ternary intermetallic ORR electrocatalyst,but also elucidates the corresponding"structure-function"relationship,which can be further applied in designing other intermetallic(electro)catalysts.