Peroxisomes are highly metabolic, autonomously replicating organelles that generate ROS as a by product of fatty acid β-oxidation. Consequently, cells must maintain peroxisome homeostasis, or risk pathologies associated with too few peroxisomes, such as peroxisome biogenesis disorders, or too many peroxisomes, inducing oxidative damage and promoting diseases such as cancer. We report that the PEX5 peroxisome import receptor binds ataxia-telangiectasia mutated (ATM) and localizes this kinase to the peroxisome. In response to reactive oxygen species (ROS), ATM signaling activates ULK1 and inhibits mTORC1 to induce autophagy. Specificity for autophagy of peroxisomes (pexophagy) is provided by ATM phosphorylation of PEX5 at Ser141, which promotes PEX5 mono-ubiquitination at K209, and recognition of ubiquitinated PEX5 by the autophagy adapter protein p62, directing the autophagosome to peroxisomes to induce pexophagy. These data reveal an important new role for ATM in metabolism as a sensor of ROS that regulates pexophagy.
Platinum (Pt) is the most active and stable HER catalyst, but its high cost and low abundance hinder its widespread applications. [3][4][5][6] Recently, tremendous efforts have been devoted to the search for noble-metal-free catalysts to replace Pt-based catalysts in the generation of H 2 with a high current density at a low overpotential. [7][8][9][10] In particularly, molybdenum carbides and molybdenum phosphides have been demonstrated as active and robust HER catalysts due to their high conductivities, high catalytic activities, and excellent stabilities. [11][12][13][14][15] The high-performance catalytic activities of these materials may be related to the function of their heteroatoms, such as phosphorus, which possesses lone-pair electrons in 3p orbitals and vacant 3d orbitals and can thus accommodate the surface charge as well as induce local charge density. [16] Nitrides of transition metals have also been shown to have excellent catalytic activities in the HER. [17][18][19][20][21] Taking all the above works together, we predicted that nitrogen (N)-doped molybdenum carbide and phosphide hybrids, N@MoPCx, might be promising electrocatalysts for efficient hydrogen evolution. However, it remains a challenge to obtain a targeted N-doped molybdenum carbide and phosphide hybrid with a uniform distribution and desirable porosity that also exhibits high electrocatalytic activity, which requires (i) preventing the aggregation of nanoparticles; (ii) obtaining a desirable porosity; and (iii) achieving uniform carburization, phosphorization, and heteroatoms doping. To avoid the aggregation of nanoparticles and increase their electrical conductivities, substrates such as carbon cloth, carbon nanotubes, and graphene have been introduced into metal-based catalysts for use in multiple catalytic reactions. [22][23][24] However, the introduction of substrates creates additional cost and still cannot completely prevent aggregation.Polyoxometalates (POMs) are a special class of well-defined molecular metal oxide clusters with a wide range of applications in medicine, catalysis, materials sciences, etc. [25][26][27][28][29][30] It is well known that organoimido derivatives of POMs can be prepared by introducing exogenous N-containing ligands to replace the oxo groups in the POM clusters. [31][32][33][34][35] The controllable preparation of multifunctionalized derivatives of hexamolybdate has been achieved by the powerful N,N′-dicyclohexylcarbodiimide (DCC)-dehydrating protocol by Ruhlmann and our group. [36,37] P-containing organoimido derivatives of POMs could be The efficient evolution of hydrogen through electrocatalysis is considered a promising approach to the production of clean hydrogen fuel. Platinum (Pt)-based materials are regarded as the most active hydrogen evolution reaction (HER) catalysts. However, the low abundance and high cost of Pt hinders the large-scale application of these catalysts. Active, inexpensive, and earth-abundant electrocatalysts to replace Pt-based materials would be highly beneficial to the ...
Bismuth vanadate (BiVO4) has been widely investigated as a photocatalyst or photoanode for solar water splitting, but its activity is hindered by inefficient cocatalysts and limited understanding of the underlying mechanism. Here we demonstrate significantly enhanced water oxidation on the particulate BiVO4 photocatalyst via in situ facet-selective photodeposition of dual-cocatalysts that exist separately as metallic Ir nanoparticles and nanocomposite of FeOOH and CoOOH (denoted as FeCoOx), as revealed by advanced techniques. The mechanism of water oxidation promoted by the dual-cocatalysts is experimentally and theoretically unraveled, and mainly ascribed to the synergistic effect of the spatially separated dual-cocatalysts (Ir, FeCoOx) on both interface charge separation and surface catalysis. Combined with the H2-evolving photocatalysts, we finally construct a Z-scheme overall water splitting system using [Fe(CN)6]3−/4− as the redox mediator, whose apparent quantum efficiency at 420 nm and solar-to-hydrogen conversion efficiency are optimized to be 12.3% and 0.6%, respectively.
Low-cost, non-noble-metal electrocatalysts are required for direct methanol fuel cells,b ut their development has been hindered by limited activity,high onset potential, low conductivity,a nd poor durability.Asurface electronic structure tuning strategy is presented, which involves doping of aforeign oxophilic post-transition metal onto transition metal aerogels to achieve an on-noble-metal aerogel Ni 97 Bi 3 with unprecedented electrocatalytic activity and durability in methanol oxidation. Trace amounts of Bi are atomically dispersed on the surface of the Ni 97 Bi 3 aerogel, which leads to an optimum shift of the d-band center of Ni, large compressive strain of Bi, and greatly increased conductivity of the aerogel. The electrocatalyst is endowed with abundant active sites, efficient electron and mass transfer,r esistance to CO poisoning, and outstanding performance in methanol oxidation. This work sheds light on the design of high-performance non-noblemetal electrocatalysts.
The in‐depth understanding of local atomic environment–property relationships of p‐block metal single‐atom catalysts toward the 2 e− oxygen reduction reaction (ORR) has rarely been reported. Here, guided by first‐principles calculations, we develop a heteroatom‐modified In‐based metal–organic framework‐assisted approach to accurately synthesize an optimal catalyst, in which single In atoms are anchored by combined N,S‐dual first coordination and B second coordination supported by the hollow carbon rods (In SAs/NSBC). The In SAs/NSBC catalyst exhibits a high H2O2 selectivity of above 95 % in a wide range of pH. Furthermore, the In SAs/NSBC‐modified natural air diffusion electrode exhibits an unprecedented production rate of 6.49 mol peroxide gcatalyst−1 h−1 in 0.1 M KOH electrolyte and 6.71 mol peroxide gcatalyst−1 h−1 in 0.1 M PBS electrolyte. This strategy enables the design of next‐generation high‐performance single‐atom materials, and provides practical guidance for H2O2 electrosynthesis.
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