The use of nitrogen fertilizers has been estimated to have supported 27% of the world’s population over the past century. Urea (CO(NH2)2) is conventionally synthesized through two consecutive ...industrial processes, N2 + H2 → NH3 followed by NH3 + CO2 → urea. Both reactions operate under harsh conditions and consume more than 2% of the world’s energy. Urea synthesis consumes approximately 80% of the NH3 produced globally. Here we directly coupled N2 and CO2 in H2O to produce urea under ambient conditions. The process was carried out using an electrocatalyst consisting of PdCu alloy nanoparticles on TiO2 nanosheets. This coupling reaction occurs through the formation of C–N bonds via the thermodynamically spontaneous reaction between *N=N* and CO. Products were identified and quantified using isotope labelling and the mechanism investigated using isotope-labelled operando synchrotron-radiation Fourier transform infrared spectroscopy. A high rate of urea formation of 3.36 mmol g–1 h–1 and corresponding Faradic efficiency of 8.92% were measured at –0.4 V versus reversible hydrogen electrode.Conventionally, urea is synthesized via two consecutive processes, N2 + H2 → NH3 followed by NH3 + CO2. Now, an electrocatalyst consisting of PdCu alloy nanoparticles on TiO2 nanosheets has been shown to directly couple N2 and CO2 in H2O to produce urea under ambient conditions.
Full text
Available for:
FZAB, GEOZS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
So far, layered PdSe2 has attracted much attention due to its completely tunable band-gap with varying layer numbers, yet the thickness-dependent transporting properties have been rarely studied. We ...have systematically studied the electronic structures, phonon and charge transport properties, and thermoelectric properties of few-layered (from 1L to 4L) and bulk PdSe2 by first-principles calculations and Boltzmann transport theory. As the thickness increases, the energy levels of band edges relative to 4s of selenium move oppositely due to their different bonding states, leading to the power-law decrease of the band-gap. Meanwhile, the electron effective mass decreases rapidly while the hole effective mass increases significantly compared with those unperturbed. Calculations on elastic constants reveal that both bulk and few-layered PdSe2 are mechanically stable, and the bulk is ductile with a Poisson's ratio of 0.27. The shifts of Raman active modes with respect to the thickness as well as their Gruneisen parameters are analyzed and the underlying physics is discussed. At room temperature, the thermal conductivities of the bulk are 7.7, 10.1 and 0.9 W m−1 K−1 along the a, b and c axes, respectively. It is found that the low-frequency modes (<2.0 THz) contribute about 80% of in-plane thermal conductivities. Due to the enhanced contribution from the ZA mode, the thermal conductivity of few-layered PdSe2 is much larger than that of the bulk. The ZA mode is mainly scattered by itself and the Umklapp scattering dominates in the process as the thickness increases. Calculations on charge transport reveal that the electron mobility increases from 2.5–13.2 (1L) to 121.9–167.8 (4L) cm2 V−1 s−1 with the decreasing anisotropy μb/μa, while the hole mobility remains to be ∼20 cm2 V−1 s−1, which is in good agreement with the experimental results. Calculations on the thermoelectric properties reveal that the ZT value as well as the power factor increases largely as the thickness increases and it gets to be optimum for the triple layer. Interestingly, the transport of electrons and phonons is decoupled along the out-of-plane direction, which makes bulk PdSe2 exhibit good thermoelectric performance along the c axis.
In recent decades, chemotherapies targeting apoptosis have emerged and demonstrated remarkable achievements. However, emerging evidence has shown that chemoresistance is mediated by impairing or ...bypassing apoptotic cell death. Several novel types of programmed cell death, such as ferroptosis, necroptosis, and pyroptosis, have recently been reported to play significant roles in the modulation of cancer progression and are considered a promising strategy for cancer treatment. Thus, the switch between apoptosis and pyroptosis is also discussed. Cancer immunotherapy has gained increasing attention due to breakthroughs in immune checkpoint inhibitors; moreover, ferroptosis, necroptosis, and pyroptosis are highly correlated with the modulation of immunity in the tumor microenvironment. Compared with necroptosis and ferroptosis, pyroptosis is the primary mechanism for host defense and is crucial for bridging innate and adaptive immunity. Furthermore, recent evidence has demonstrated that pyroptosis exerts benefits on cancer immunotherapies, including immune checkpoint inhibitors (ICIs) and chimeric antigen receptor T-cell therapy (CAR-T). Hence, in this review, we elucidate the role of pyroptosis in cancer progression and the modulation of immunity. We also summarize the potential small molecules and nanomaterials that target pyroptotic cell death mechanisms and their therapeutic effects on cancer.
This study evaluated short-term (1-month) and long-term (1-year) mortality risks associated with the glomerular filtration rate (eGFR) on admission for patients with intracerebral hemorrhage.
From ...the Taiwan Stroke Registry data from April 2006 to December 2016, we identified and stratified patients with intracerebral hemorrhage into five subgroups by the eGFR level on admission: ≥90, 60-89, 30-59, 15-29, and <15 mL/min/1.73 m2 or on dialysis. Risks for 1-month and 1-year mortality after intracerebral hemorrhage were compared by the eGFR levels.
Both the 1-month and 1-year mortality rates progressively increased with the decrease in eGFR levels. The 1-month mortality rate in patients with eGFR < 15 mL/min/1.73 m2 or on dialysis was approximately 5.5-fold greater than that in patients with eGFR ≥ 90 mL/min/1.73 m2 (8.31 versus 1.50 per 1000 person-days), with an adjusted hazard ratio (HR) of 4.59 95% confidence interval (CI) = 2.71-7.78. Similarly, the 1-year mortality in patients with eGFR < 15 mL/min/1.73 m2 or on dialysis was 7.5 times that in patients with eGFR ≥ 90 mL/min/1.73 m2 (2.34 versus 0.31 per 1000 person-days), with an adjusted HR of 4.54 (95% CI 2.95-6.98).
Impairment of renal function is an independent risk factor for mortality in patients with intracerebral hemorrhage in a gradual way. The eGFR level is a prognostic indicator for patients with intracerebral hemorrhage.
Full text
Available for:
DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Sensory neurons are distinguished by distinct signaling networks and receptive characteristics. Thus, sensory neuron types can be defined by linking transcriptome-based neuron typing with the sensory ...phenotypes. Here we classify somatosensory neurons of the mouse dorsal root ganglion （DRG） by high-coverage single-cell RNA-sequencing （10 950 ±1 218 genes per neuron） and neuron size-based hierarchical clustering. Moreover, single DRG neurons responding to cutaneous stimuli are recorded using an in vivo whole-cell patch clamp technique and classified by neuron-type genetic markers. Small diameter DRG neurons are classified into one type of low-threshold mechanoreceptor and five types of mechanoheat nociceptors （MHNs）. Each of the MHN types is further categorized into two subtypes. Large DRG neurons are categorized into four types, including neurexophilin 1-expressing MHNs and mechanical nociceptors （MNs） expressing BAil-associated protein 2-like I （Baiap211）. Mechanoreceptors expressing trafficking protein particle complex 3-like and Baiap211-marked MNs are subdivided into two subtypes each. These results provide a new system for cataloging somatosensory neurons and their transcriptome databases.
Full text
Available for:
EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
Kinetically stable and long‐lived intermediates are crucial in monitoring the progress and understanding of supramolecular self‐assembly of diverse aggregated structures with collective functions. ...Herein, the complex dynamics of an atomically precise CuI nanocluster Cu8(tBuC6H4S)8(PPh3)4 (Cu8a) is systematically investigated. Remarkably, by monitoring the aggregation‐induced emission (AIE) and electron microscopy of the kinetically stable intermediates in real time, the directed self‐assembly (DSA) process of Cu8a is deduced. The polymorphism and different emission properties of Cu NCs aggregates were successfully captured, allowing the structure–optical property relationship to be established. More importantly, the utilization of a mathematical “permutation and combination” ideology by introducing a heterogeneous luminescent agent of a carbon dot (CD) to Cu8a aggregates enriches the “visualization” fluorescence window, which offers great potential in real time application for optical sensing of materials.
Within the scheme of aggregation‐induced emission (AIE), optical‐engineering was performed for real‐time monitoring of the self‐assembly process of Cu8a with various kinetic long‐lived intermediates, leading to a structure–property relationship being established.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Sonodynamic therapy (SDT) has rapidly developed as a powerful alternative to traditional photodynamic therapy due to its intrinsically deeper tissue-penetration. However, single SDT dose is incapable ...of radical cure because the long-term hypoxia of tumor limits its therapeutic effect. Herein, we developed a biomimetic nanoplatform with dual pH/ultrasound response, homologous targeting and low phototoxicity for combined nitric oxide (NO) gas therapy with SDT to solve the problem. This nanoplatform is composed of zeolite imidazole framework-8 material embedded with nitrosoglutathione (GSNO) and chlorin e6 (Ce6) by one-step encapsulation, and then wrapped by homologous tumor cell membrane. In vitro and in vivo experiments indicate that the biomimetic nanoplatform has excellent biocompatibility and shows higher retention in tumor by homologous targeting. Importantly, it can sustainably release the encapsulated drug in acidic tumor microenvironment and accelerate degradation by ultrasound (US). Furthermore, NO released from GSNO and reactive oxygen species generated by Ce6, which are both triggered by US, react with each other to produce highly reactive peroxynitrite to inhibit the growth of tumor. Moreover, by repeated US irradiation, the tumor hypoxia can be relieved for a much-longer term, resulting in an effective gas-sonodynamic combined treatment. This study fully utilizes the advantages of US, providing a new strategy for high-performance cancer therapy.
Full text
Available for:
GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
A model-free predictive current control (PCC) of interior permanent-magnet synchronous motor (IPMSM) drive systems based on a current difference detection technique is proposed. The model-based PCC ...(MBPCC) of IPMSM requires knowledge of parameters such as resistance, q-axis inductance, and extended back EMF. This paper develops a new model-free approach that alleviates the need for excessive prior knowledge about the system and only utilizes the stator currents as well as the current differences corresponding to different switching states of the inverter. Despite the salient difference of the proposed approach, it adopts a measure similar to that in the MBPCC approach to obtain the next switching state of the inverter by minimizing a cost function. It is noteworthy that the proposed method is easy to implement due to its simplicity and free of any multiplication operation. For comparison purposes, a digital signal processor, TMS320LF2407, is used to execute the two aforementioned current control techniques. Several experimental results show that the proposed method can significantly improve the current-tracking performance.
A
bstract
A coupling of a dark photon
A
′
from a U(1)
A
′ with the standard model (SM) particles can be generated through kinetic mixing represented by a parameter
ϵ
. A non-zero ϵ also induces a ...mixing between
A
′
and
Z
if dark photon mass
m
A
′ is not zero. This mixing can be large when
m
A
′ is close to
m
Z
even if the parameter
ϵ
is small. Many efforts have been made to constrain the parameter
ϵ
for a low dark photon mass
m
A
′ compared with the
Z
boson mass
m
Z
. We study the search for dark photon in
e
+
e
−
→ γ
A
′
→ γ
μ
+
μ
−
for a dark photon mass
m
A
′ as large as kinematically allowed at future
e
+
e
−
colliders. For large
m
A
′, care should be taken to properly treat possible large mixing between
A
′
and
Z
. We obtain sensitivities to the parameter
ϵ
for a wide range of dark photon mass at planed
e
+
e
−
colliders, such as Circular Electron Positron Collider (CEPC), International Linear Collider (ILC) and Future Circular Collider (FCC-ee). For the dark photon mass 20 GeV ≲
m
A
′ ≲ 330 GeV, the 2
σ
exclusion limits on the mixing parameter are
ϵ
≲ 10
−3
-10
−2
. The CEPC with
s
=
240
GeV and FCC-ee with
s
=
160
GeV are more sensitive than the constraint from current LHCb measurement once the dark photon mass
m
A
′ ≳ 50 GeV. For
m
A
′ ≳ 220 GeV, the sensitivity at the FCC-ee with
s
=
350
GeV and 1
.
5 ab
−1
is better than that at the 13 TeV LHC with 300 fb
−1
, while the sensitivity at the CEPC with
s
=
240
GeV and 5ab
−1
can be even better than that at 13TeV LHC with 3ab
−1
for
m
A
′ ≳ 180 GeV. We also comment on sensitivities of
e
+
e
−
→ γ
A
′
with dark photon decay into several other channels at future
e
+
e
−
colliders.
This is a retrospective cohort study by analyzing a multi‐institutional electronic medical records database in Taiwan to compare long‐term effectiveness and risk of major adverse cardiac events ...(MACE) in chemotherapy‐naïve metastatic castration‐resistant prostate cancer (mCRPC) patients treated with enzalutamide (ENZ) or abiraterone (AA). Patients aged 20 years and older and newly receiving androgen receptor targeted therapies ENZ or AA from September 2016 to December 2019 were included. We followed patients from initiation of therapies to the occurrence of outcomes (prostate‐specific antigen (PSA) response rate, PSA progression free survival (PFS), overall survival (OS), and MACE), death, the last clinical visit, or December 31, 2020. We performed multivariable Cox proportional hazard models to compare ENZ and AA groups for the measured outcomes. A total of 363 patients treated with either ENZ (n = 157) or AA (n = 206) were identified. The analysis found a significantly higher proportion of patients with a PSA response rate higher than 50% among those receiving ENZ than among those receiving AA (ENZ vs AA: 75.80% vs 63.59%, P = .01). However, there was no significant difference in PSA PFS (adjusted hazard ratio: 0.86; 95% CI 0.63‐1.17) and OS (0.68: 0.41‐1.14) between the use of ENZ and AA in chemotherapy‐naïve mCRPC patients. Regarding the cardiovascular (CV) safety outcome, there was a significantly lower risk of MACE in patients receiving ENZ, compared to patients receiving AA (0.20: 0.07‐0.55). The findings suggest that enzalutamide may be more efficacious for PSA response and suitable for chemotherapy‐naïve mCRPC patients with high CV risk profile.
What's new?
While second generation androgen receptor (AR)‐targeted therapies are promising for the treatment of chemotherapy‐naïve metastatic castration‐resistant prostate cancer (mCRPC), data on survival benefit and cardiovascular safety are lacking. Here, using a multi‐institutional electronic health records database, the authors investigated the effectiveness, long‐term outcome, and cardiovascular safety of the AR‐targeted mCRPC therapies enzalutamide and abiraterone. Compared to abiraterone, enzalutamide is more efficacious in terms of prostate‐specific antigen response and carries a lower risk of major adverse cardiac events. The findings are relevant for treatment decisions regarding AR‐targeted therapies for chemotherapy‐naïve mCRPC patients with high risk of adverse cardiovascular events.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
PDF
