Metal bond strength regulation enables large-scale synthesis of intermetallic nanocrystals for practical fuel cells.

Structurally ordered L10-PtM (M = Fe, Co, Ni and so on) intermetallic nanocrystals, benefiting from the chemically ordered structure and higher stability, are one of the best electrocatalysts used for fuel cells. However, their practical development is greatly plagued by the challenge that the high-temperature (>600 °C) annealing treatment necessary for realizing the ordered structure usually leads to severe particle sintering, morphology change and low ordering degree, which makes it very difficult for the gram-scale preparation of desirable PtM intermetallic nanocrystals with high Pt content for practical fuel cell applications. Here we report a new concept involving the low-melting-point-metal (M' = Sn, Ga, In)-induced bond strength weakening strategy to reduce Ea and promote the ordering process of PtM (M = Ni, Co, Fe, Cu and Zn) alloy catalysts for a higher ordering degree. We demonstrate that the introduction of M' can reduce the ordering temperature to extremely low temperatures (≤450 °C) and thus enable the preparation of high-Pt-content (≥40 wt%) L10-Pt-M-M' intermetallic nanocrystals as well as ten-gram-scale production. X-ray spectroscopy studies, in situ electron microscopy and theoretical calculations reveal the fundamental mechanism of the Sn-facilitated ordering process at low temperatures, which involves weakened bond strength and consequently reduced Ea via Sn doping, the formation and fast diffusion of low-coordinated surface free atoms, and subsequent L10 nucleation. The developed L10-Ga-PtNi/C catalysts display outstanding performance in H2-air fuel cells under both light- and heavy-duty vehicle conditions. Under the latter condition, the 40% L10-Pt50Ni35Ga15/C catalyst delivers a high current density of 1.67 A cm-2 at 0.7 V and retains 80% of the current density after extended 90,000 cycles, which exceeds the United States Department of Energy performance metrics and represents among the best cathodic electrocatalysts for practical proton-exchange membrane fuel cells.

PdMo bimetallene for oxygen reduction catalysis.

The efficient interconversion of chemicals and electricity through electrocatalytic processes is central to many renewable-energy initiatives. The sluggish kinetics of the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER)1-4 has long posed one of the biggest challenges in this field, and electrocatalysts based on expensive platinum-group metals are often required to improve the activity and durability of these reactions. The use of alloying5-7, surface strain8-11 and optimized coordination environments12 has resulted in platinum-based nanocrystals that enable very high ORR activities in acidic media; however, improving the activity of this reaction in alkaline environments remains challenging because of the difficulty in achieving optimized oxygen binding strength on platinum-group metals in the presence of hydroxide. Here we show that PdMo bimetallene-a palladium-molybdenum alloy in the form of a highly curved and sub-nanometre-thick metal nanosheet-is an efficient and stable electrocatalyst for the ORR and the OER in alkaline electrolytes, and shows promising performance as a cathode in Zn-air and Li-air batteries. The thin-sheet structure of PdMo bimetallene enables a large electrochemically active surface area (138.7 square metres per gram of palladium) as well as high atomic utilization, resulting in a mass activity towards the ORR of 16.37 amperes per milligram of palladium at 0.9 volts versus the reversible hydrogen electrode in alkaline electrolytes. This mass activity is 78 times and 327 times higher than those of commercial Pt/C and Pd/C catalysts, respectively, and shows little decay after 30,000 potential cycles. Density functional theory calculations reveal that the alloying effect, the strain effect due to the curved geometry, and the quantum size effect due to the thinness of the sheets tune the electronic structure of the system for optimized oxygen binding. Given the properties and the structure-activity relationships of PdMo metallene, we suggest that other metallene materials could show great promise in energy electrocatalysis.

Complex association of body mass index and outcomes in patients with relapsed and refractory multiple myeloma treated with CAR-T cell immunotherapy.

BACKGROUND AIMS: Chimeric antigen receptor-T (CAR-T) cells have exhibited remarkable efficacy in treating refractory or relapsed multiple myeloma (R/R MM). Although obesity has a favorable value in enhancing the response to immunotherapy, less is known about its predictive value regarding the efficacy and prognosis of CAR-T cell immunotherapy. METHODS: We conducted a retrospective study of 111 patients with R/R MM who underwent CAR-T cell treatment. Using the body mass index (BMI) classification, the patients were divided into a normal-weight group (73/111) and an overweight group (38/111). We investigated the effect of BMI on CAR-T cell therapy outcomes in patients with R/R MM. RESULTS: The objective remission rates after CAR-T cell infusion were 94.7% and 89.0% in the overweight and normal-weight groups, respectively. The duration of response and overall survival were not significant difference between BMI groups. Compared to normal-weight patients, overweight patients had an improved median progression-free survival. There was no significant difference in cytokine release syndrome and immune effector cell-associated neurotoxicity syndrome between the subgroups. In terms of hematological toxicity, the erythrocyte, hemoglobin, platelet, leukocyte and neutrophil recovery was accelerated in the overweight group. Fewer patients in the overweight group displayed moderate percent CD4 and CD4/CD8 ratios compared to the normal-weight group. Furthermore, the percent CD4 ratios were positively correlated with the levels of cytokines [interleukin-2 (IL-2) (day 14), interferon gamma (IFN-γ) (day 7) and tumor necrosis factor alpha (TNF-α) (days 14 and 21)] after cells infusion. On the other hand, BMI was positively associated with the levels of IFN-γ (day 7) and TNF-α (days 14 and 21) after CAR-T cells infusion. CONCLUSIONS: Overall, this study highlights the potential beneficial effect of a higher BMI on CAR-T cell therapy outcomes.

Reason and control strategy for denitrification and anammox sludge flotation in nitrogen removal process: Mechanisms, strategies and perspectives.

Anaerobic biological treatment technology, especially denitrification and anaerobic ammonia oxidation (anammox) technology as mainstream process, played dominant role in the field of biological wastewater treatment. However, the above process was prone to sludge floating during high load operation and thereby affecting the efficient and stable operation of the system. Excessive production of extracellular polymeric substance (EPS) was considered to be the main reason for anaerobic granular sludge flotation, but the summaries in this area were not comprehensive enough. In this review, the potential mechanisms of denitrification and anammox sludge floatation were discussed from the perspective of granular sludge structural characteristics, nutrient transfer, and microbial flora change respectively, and the corresponding control strategies were also summarized. Finally, this paper indicated that future research on sludge flotation should focus on reducing the negative effects of EPS in sludge particles.

Low-Electronegativity Mn-Contraction of PtMn Nanodendrites Boosts Oxygen Reduction Durability.

Platinum metal (PtM, M=Ni, Fe, Co) alloys catalysts show high oxygen reduction reaction (ORR) activity due to their well-known strain and ligand effects. However, these PtM alloys usually suffer from a deficient ORR durability in acidic environment as the alloyed metal is prone to be dissolved due to its high electronegativity. Herein, we report a new class of PtMn alloy nanodendrite catalyst with low-electronegativity Mn-contraction for boosting the oxygen reduction durability of fuel cells. The moderate strain in PtMn, induced by Mn contraction, yields optimal oxygen reduction activity at 0.53 A mg-1 at 0.9 V versus reversible hydrogen electrode (RHE). Most importantly, we show that relative to well-known high-electronegativity Ni-based Pt alloy counterpart, the PtMn nanodendrite catalyst experiences less transition metals' dissolution in acidic solution and achieves an outstanding mass activity retention of 96 % after 10,000 degradation cycles. Density functional theory calculation reveals that PtMn alloys are thermodynamically more stable than PtNi alloys in terms of formation enthalpy and cohesive energy. The PtMn nanodendrite-based membrane electrode assembly delivers an outstanding peak power density of 1.36 W cm-2 at a low Pt loading and high-performance retention over 50 h operations at 0.6 V in H2 -O2 hydrogen fuel cells.

High Valence M-Incorporated PdCu Nanoparticles (M = Ir, Rh, Ru) for Water Electrolysis in Alkaline Solution.

The high-valence metal catalysts show extraordinary talent in various electrochemical reactions. However, there is no facile method to synthesize high-valence noble metal-based materials. Herein, we synthesized the different high valence noble metal M-incorporated PdCu nanoparticles (M = Ir, Ru, Rh) by the assistant of Fe3+ and exhibit excellent performance for water electrolysis. In 0.1 M KOH, the OER and HER mass activities of Ir16-PdCu/C were 50.5 and 16.5 times as much as PdCu/C, and achieved a current density of 10 mA cm-2 at 1.63 V when worked for overall water splitting. DFT calculation revealed that the incorporating of high valence Ir could optimize the binding energy of the intermediate products, and promote the evolution of oxygen and hydrogen. Ex situ XPS shows that the huge amount of oxidized Ir (V) formed in OER could promote the formation of O-O bonds.

A Unique Gas-Migration, Trapping, and Emitting Strategy for High-Loading Single Atomic Cd Sites for Carbon Dioxide Electroreduction.

Single-atom catalysts (SACs) exhibit great potential in heterogeneous catalysis. However, the achievement of obtaining high-loading SACs remains a bottleneck. Herein, we first demonstrate a unique gas-migration, trapping, and emitting strategy for building a kind of Cd-based SAC for CO2 reduction (CO2RR). The gas-migration and trapping processes (≤750 °C) endows the material with an ultrahigh Cd loading amount of 30.3 wt %, while the emitting process can facilely modulate the loading amount from 30.3 to 1.4 wt %. For the CO2RR, the Cd-NC SACs with a loading amount of 18.4 wt % exhibits the maximum Faraday efficiency of 91.4% for CO at -0.728 V. The operando infrared spectroscopy studies prove the presence of main intermediates *COO-, *COOH, and *CO on Cd-NC-5M SACs during the catalytic process, indicating that the CO2RR follows the proton-decoupled electron-transfer mechanism. Density functional theory simulations reveal that the Cd-N4 structure reduces the Gibbs free energy of the rate-determining step (the hydrogenation step of *COOH).

Interfacial Engineering in PtNiCo/NiCoS Nanowires for Enhanced Electrocatalysis and Electroanalysis.

Searching for new anti-poisoning Pt-based catalysts with enhanced activity for alcohol oxidation is the key in direct alcohol fuel cells (DAFCs). However, in the traditional strategy for designing bimetallic or multimetallic alloy is still difficult to achieve a satisfactory heterogeneous electrocatalyst because the activity often depends on only the surface atoms. Herein, we fabricate the multicomponent active sites by creating a sulfide structure on 1D PtNiCo trimetallic nanowires (NWs), to give a PtNiCo/NiCoS interface NWs (IFNWs). Owing to the presence of sulfide interfaces, the PtNiCo/NiCoS IFNWs enable an impressive methanol/ethanol oxidation reaction (MOR/EOR) performance and excellent anti-CO poisoning tolerance. They have the MOR and EOR mass activities of 2.25 Amg-1 Pt and 1.62 Amg-1 Pt , around 1.26, 3.21 and 1.46, 2.96 times higher than those of PtNiCo NWs and commercial Pt/C, respectively. CO-stripping and XPS measurements further demonstrate that the new interfacial structure and optimal bonding of Pt-CO can result in accelerating the removal of surface adsorbed carbonaceous intermediates. Moreover, such a unique structure has also demonstrated a much-improved ability for the electrochemical detection of some important molecules (H2 O2 and NH2 NH2 ).

Evolutionary and recombination analysis of porcine reproductive and respiratory syndrome isolates in China.

Seven strains of porcine reproductive and respiratory syndrome virus (PRRSV) were isolated from 2014 to 2017 in the Shandong province of China and their genomes were sequenced and analyzed. Results showed that all seven of the isolates belong to PRRSV 2, and are clustered into four lineages (lineage 1, 3, 5 and 8) based on comparisons of the ORF5 gene. Comparative analysis of genomes and specific amino acid sites revealed that three of the strains (SDwh1402, SDwh1602 and SDwh1701) have evolved directly from modified live virus (MLV) JXA1-P80, TJM-F92 and IngelvacPRRS. Further recombination analysis revealed that two of the strains (SDyt1401 and SDwh1601) were the result of a recombination event between MLVs JXA1-P80 and NADC30 while two other strains (SDwh1403 and SDqd1501) were the result of recombination between MLVs IngelvacPRRS and NADC30 and HP-PRRSV and QYYZ, respectively. Our results add to the data on MLV evolution and PRRSV recombination and provide a better understanding of the epidemiology of PRRSV in China.

Correction to: Evolutionary and recombination analysis of porcine reproductive and respiratory syndrome isolates in China.

The original version of this article unfortunately contained an error in GenBank Accession Number.

Multimetal Borides Nanochains as Efficient Electrocatalysts for Overall Water Splitting.

The development of cost-efficient, active, and stable electrode materials as bifunctional catalysts for electrochemical water splitting is crucial to high-performance renewable energy storage and conversion devices. In this work, the synthesis of Co-based multi-metal borides nanochains with amorphous structure is reported for boosting the oxygen evolution (OER) and hydrogen evolution reactions (HER) by one-pot NaBH4 reduction of Co2+ , Ni2+ , and Fe2+ under ambient temperature. In all the investigated Co-based metal borides, NiCoFeB nanochains show the excellent OER performance with a low overpotential of 284 mV at 10 mA cm-2 and Tafel slope of 46 mV dec-1 , respectively, together with excellent catalytic stability, and robust HER performance with an overpotential of 345 mV at 10 mA cm-2 . The density functional theory (DFT) calculations reveal that the excellent electrocatalytic performance is mainly attributed to optimal electronic structure by tuning the Co-3d band activities by the incorporation of Ni and Fe for enhanced water splitting via the potentially existed Co0 state. Moreover, the electrolyzer using NiCoFeB nanochains as anode and cathode offers 10 mA cm-2 at a cell voltage of 1.81 V, comparable to commercial Pt/C // Ir/C, providing a simple method to design and explore highly efficient and cheap bifunctional electrocatalysts for overall water splitting.

Butyphthalide in the treatment of massive Cerebral Infarction.

OBJECTIVE: To evaluate the effect of butyphthalide in the treatment of massive cerebral infarction. METHODS: One hundred and twenty patients with massive cerebral infarction who were admitted to the hospital between January 2017 and December 2017 were selected and divided into a treatment group (n = 60) and a control group (n = 60) using random number table, 80 each group. Patients in the control group were given conventional cerebral infarction therapy, while patients in the treatment group were given butyphthalide injection besides the conventional treatment. The National Institutes of Health Stroke Scale (NIHSS) score, score of activity of daily living (ADL), lipoprotein-associated phospholipase A2 (LP-PLA2) and prognosis were recorded and compared between the two groups. The response rates of the two groups were recorded. RESULTS: The total response rates of the control group and treatment group were 73.85% and 93.85% respectively at the postoperative 21st day, and the difference had statistical significance (P<0.05). The NIHSS score of the two groups obviously decreased, and the ADL score significantly increased after treatment; the differences of NIHSS score and ADL score before and after treatment in the same group had statistical significance (P<0.05). The improvement of the indexes of the treatment group was obviously superior to that of the control group, and the differences between the two groups had statistical significance (P<0.05). The level of LP-PLA2 of both groups significantly decreased at the postoperative 21st day, and the difference before and after treatment in the same group was statistically significant (P<0.05); the treatment group had a significantly lower level of LP-PLA2 than the control group, and the difference had statistical significance (P<0.05). The treatment group had significantly higher positive outcome rate and lower mortality rate than the control group at the postoperative 90th day, and the differences had statistical significance (P<0.05). The incidence of adverse events of the treatment group and control group was 8.3% (5/60) and 5.0% (3/60) respectively, suggesting no significant difference (P>0.05). CONCLUSION: Butyphthalide has a favourable effect in treating massive cerebral infarction. It can repair neurologic impairment, improve activity of daily living, and adjust the level of LP-PLA2, suggesting favourable application values.

The Kirkendall Effect for Engineering Oxygen Vacancy of Hollow Co3 O4 Nanoparticles toward High-Performance Portable Zinc-Air Batteries.

Structure and defect control are widely accepted effective strategies to manipulate the activity and stability of catalysts. On a freestanding hierarchically porous carbon microstructure, the tuning of oxygen vacancy in the embedded hollow cobaltosic oxide (Co3 O4 ) nanoparticles is demonstrated through the regulation of nanoscale Kirkendall effect. Starting with the embedded cobalt nanoparticles, the concentration of oxygen-vacancy defect can vary with the degree of Kirkendall oxidation, thus regulating the number of active sites and the catalytic performances. The optimized freestanding catalyst shows among the smallest reversible oxygen overpotential of 0.74 V for catalyzing oxygen reduction/evolution reactions in 0.1 m KOH. Moreover, the catalyst shows promise for substitution of noble metals to boost cathodic oxygen reactions in portable zinc-air batteries. This work provides a strategy to explore catalysts with controllable vacancy defects and desired nano-/microstructures.

Defects and Interfaces on PtPb Nanoplates Boost Fuel Cell Electrocatalysis.

Nanostructured Pt is the most efficient single-metal catalyst for fuel cell technology. Great efforts have been devoted to optimizing the Pt-based alloy nanocrystals with desired structure, composition, and shape for boosting the electrocatalytic activity. However, these well-known controls still show the limited ability in maximizing the Pt utilization efficiency for achieving more efficient fuel cell catalysis. Herein, a new strategy for maximizing the fuel cell catalysis by controlling/tuning the defects and interfaces of PtPb nanoplates using ion irradiation technique is reported. The defects and interfaces on PtPb nanoplates, controlled by the fluence of incident C+ ions, make them exhibit the volcano-like electrocatalytic activity for methanol oxidation reaction (MOR), ethanol oxidation reaction (EOR), and oxygen reduction reaction (ORR) as a function of ion irradiation fluence. The optimized PtPb nanoplates with the mixed structure of dislocations, subgrain boundaries, and small amorphous domains are the most active for MOR, EOR, and ORR. They can also maintain high catalytic stability in acid solution. This work highlights the impact and significance of inducing/controlling the defects and interfaces on Pt-based nanocrystals toward maximizing the catalytic performance by advanced ion irradiation strategy.

Graphene/Intermetallic PtPb Nanoplates Composites for Boosting Electrochemical Detection of H2O2 Released from Cells.

Rational design and construction of electrocatalytic nanomaterials is vital for improving the sensitivity and selectivity of nonenzymatic electrochemical sensors. Here, we report a novel graphene supported intermetallic PtPb nanoplates (PtPb/G) nanocomposite as an enhanced electrochemical sensing platform for high-sensitivity detection of H2O2 in neutral solution and also released from the cells. The intermetallic PtPb nanoplates are first synthesized via a simple wet-chemistry process and subsequently assembled on graphene via a solution-phase self-assembly approach. The obtained nanocomposite exhibits excellent electrocatalytic activity for the electrochemical reduction of H2O2 in a half-cell test and can detect H2O2 with a wide linear detection range of 2 nM to 2.5 mM and a very low detection limit of 2 nM. Under the same conditions, the sensitivity of PtPb/G for the detection of H2O2 is more than 12.7 times higher than that of commercial Pt/C. The high-density of electrocatalytic active sites on the unique PtPb nanoplates and the synergistic effect between PtPb nanoplates and graphene appear to be the main factors in contributing to the outstanding electroanalytical performance. The PtPb/G can be also used for the practical detection of H2O2 released from Raw 264.7 cells.

Identification of a linear B-cell epitope on the avian leukosis virus P27 protein using monoclonal antibodies.

Avian leukosis virus (ALV) is an avian oncogenic retrovirus that can induce various clinical tumors. The capsid protein P27 is the group-specific antigen of ALV and has many viral antigen sites that are easy to detect. In this study, we produced a monoclonal antibody (mAb), 3A9, that is specific for the P27 protein. A series of partially overlapping peptides were screened to define (181)PPSAR(185) as the minimal linear epitope recognized by mAb 3A9. The identified epitope could be recognized by chicken anti-ALV and mouse anti-ALV P27 sera. The epitope was highly conserved among a number of ALV-A, ALV-B and ALV-J strains. MAb 3A9 might be a valuable tool for the development of new immunodiagnostic approaches for ALV, and the defined linear epitope might help further our understanding of the antigenic structure of the P27 protein.

Rapid detection of highly pathogenic porcine reproductive and respiratory syndrome virus by a fluorescent probe-based isothermal recombinase polymerase amplification assay.

A novel fluorescent probe-based real-time reverse transcription recombinase polymerase amplification (real-time RT-RPA) assay was developed for rapid detection of highly pathogenic type 2 porcine reproductive and respiratory syndrome virus (HP-PRRSV). The sensitivity analysis showed that the detection limit of RPA was 70 copies of HP-PRRSV RNA/reaction. The real-time RT-RPA highly specific amplified HP-PRRSV with no cross-reaction with classic PRRSV, classic swine fever virus, pseudorabies virus, and foot-and-mouth disease virus. Assessment with 125 clinical samples showed that the developed real-time RT-RPA assay was well correlated with real-time RT-qPCR assays for detection of HP-PRRSV. These results suggest that the developed real-time RT-RPA assay is suitable for rapid detection of HP-PRRSV.

Characterization and energy potential of food waste from catering service in Hangzhou, China.

Safe disposal of food waste is becoming an impending issue in China with the rapid increase of its production and the promotion of environmental awareness. Food waste from catering services in Hangzhou, China, was surveyed and characterized in this study. A questionnaire survey involving 632 units across the urban districts showed that 83.5% of the food waste was not properly treated. Daily food waste production from catering units was estimated to be 1184.5 tonnes. The ratio of volatile solid to total solid, easily biodegradable matter (including crude fat, crude protein and total starch) content in total solid and the ratio of total organic carbon to nitrogen varied in ranges of 90.1%-93.9%, 60.9%-72.1%, and 11.9-19.9, respectively. Based on the methane yield of 350 mL g VS(-1) in anaerobic batch tests, annual biogas energy of 1.0 × 10(9) MJ was estimated to be recovered from the food waste. Food waste from catering services was suggested to be an attractive clean energy source by anaerobic digestion.

Assessing spatiotemporal risks of nonpoint source pollution via soil erosion: a coastal case in the Yellow River Delta, China.

Nonpoint source pollution (NPSP) has always been the dominant threat to regional waters. Based on empirical models of the revised universal soil loss equation and the phosphorus index, an NPSP risk assessment model denoted as SL-NPSRI was developed. The surface soil pollutant loss was estimated by simulating the rain-runoff topographic process, and the influence of path attenuation was quantified. A case study in the Yellow River Delta and corresponding field surveys of soil pollutants and water quality showed that the established model can be applied to evaluate the spatial heterogeneity of NPSP. NPSP usually occurs during high-intensity rainfall periods and in larger estuaries. Summer rainfall increased pollutant transport into the sea from late July to mid-August and caused estuarine dilution. Higher NPSP risks often correspond to coastal areas with lower vegetation coverage, higher soil erodibility, and higher soil pollutant concentrations. Agricultural NPSP originating from cropland significantly increase the pollutant fluxes. Therefore, area-specific land use management and vegetation coverage improvement, and temporal-specific strategies can be explored for NPSP control during source-transport hydrological processes. This research provides a novel insight for coastal NPSP simulations by comprehensively analyzing the soil erosion process and its associated pollutant loss effects, which can be useful for targeted spatiotemporal solutions.

Assembled RhRuFe Trimetallene for Water Electrolysis.

Industrializing water electrolyzers demands better electrocatalysts, especially for the anodic oxygen evolution reaction (OER). The prevailing OER catalysts are Ir or Ru-based nanomaterials, however, they still suffer from insufficient stability. An alternative yet considerably less explored approach is to upgrade Rh, a known stable but moderately active element for OER electrocatalysis, via rational structural engineering. Herein, a precise synthesis of assembled RhRuFe trimetallenes (RhRuFe TMs) with an average thickness of 1 nm for boosting overall water splitting catalysis is reported. Favorable mass transport and optimized electronic structure collectively render RhRuFe TMs with an improved OER activity of an overpotential of 330 mV to deliver 10 mA cm-2, which is significantly lower than the Rh/C control (by 601 mV) and reported Rh-based OER electrocatalysts. In particular, the RhRuFe TMs-based water splitting devices can achieve the current density of 10 mA cm-2 at a low voltage of 1.63 V, which is among the best in the Rh-based bifunctional catalysts for electrolyzers. The addition of Fe in RhRuFe TMs can modulate the strain/electron distribution of the multi-alloy, which regulates the binding energies of H* and OH* in hydrogen and oxygen evolution reactions for achieving the enhanced bifunctional OER and HER catalysis is further demonstrated.