Herein,we couple a synthetic electrozyme in a supramolecule-assembled nanoarchitecture to achieve enhanced bioenergy transformation by mimicking mitochondrial oxidative phosphorylation.Different from the natural count...Herein,we couple a synthetic electrozyme in a supramolecule-assembled nanoarchitecture to achieve enhanced bioenergy transformation by mimicking mitochondrial oxidative phosphorylation.Different from the natural counterpart,the metal-free electrozyme is a semiconducting polymer deposited on an electrode.The wellmatched electrocatalytic property of the electrozyme permits oxidization of reduced nicotinamide adenine dinucleotide(NADH)to release protons under a much lower electric potential.As a consequence,the generated proton gradient drives rotary catalysis of adenosine 5′-triphosphate(ATP)synthase reconstituted in a lipid membrane to produce ATP.Remarkably,electrochemical bioenergy conversion of NADH to ATP is accomplished with much higher efficiency in such a bio-like system compared with the natural mitochondria.This work integrates synthetic and natural catalytic chemistry to facilitate enhanced bioenergy transformation,thereby greatly improving prospects in ATP-fueled bioapplications.展开更多
The manipulation of supramolecular assembly enables single-component architectures to possess diverse structures and functions.Here,we report directed phase transitions of dipeptide supramolecular gel to crystals with...The manipulation of supramolecular assembly enables single-component architectures to possess diverse structures and functions.Here,we report directed phase transitions of dipeptide supramolecular gel to crystals with excellent selectivity and tunable mechanical properties.To be specific,lamellar-to-orthorhombic rearrangement of dipeptide molecules in the supramolecular assembly was guided by application of ammonia gas,while lamellar-tohexagonal realignment was generated upon water vapor exposure of the assembly.Importantly,this crystal phase control originated from distinct gas-mediated reconstitution of hydrogen-bonding interactions,which endowed the dipeptide materials with remarkably modulated stiffness.The selective phase transformation offers a simple and effective platform for self-assembling peptide crystals with diverse long-range-ordered structures from a single gel-state aggregation.This work opens up new perspectives on peptide-based biomaterials via gas-directed hydrogen-bonding chemistry.展开更多
We construct a natural-artificial hybrid architecture containing black phosphorus nanosheets(BPNS)to enhance photosynthesis of chloroplast in a positive-feedback manner.In this architecture,oxygen yielded by photosynt...We construct a natural-artificial hybrid architecture containing black phosphorus nanosheets(BPNS)to enhance photosynthesis of chloroplast in a positive-feedback manner.In this architecture,oxygen yielded by photosynthesis during water splitting by photosystemⅡpromotes the photoreaction of BPNS to produce proton and inorganic phosphate(Pi).Further,transmembrane proton gradient is increased to drive ATP synthase to synthesize ATP.Meanwhile,additional photogenerated electrons produced by BPNS are transferred to the photosynthesis process.As a consequence,photosynthesis performed by chloroplast is improved.Quantitatively,photophosphorylation efficacy of the hybrid system is increased by 1.89 times in the case of Pi deficiency.This work offers a new path to enhance solar-to-chemical energy conversion,holding promise in boosting natural photosynthesis.展开更多
基金This work was supported by the NationalNatural Science Foundation of China(grant nos.221930301,21961142022,22072160,and 21872150).J.F.particularly thanks to Institute of Chemistry,CAS(grant no.Y6290512B1).
文摘Herein,we couple a synthetic electrozyme in a supramolecule-assembled nanoarchitecture to achieve enhanced bioenergy transformation by mimicking mitochondrial oxidative phosphorylation.Different from the natural counterpart,the metal-free electrozyme is a semiconducting polymer deposited on an electrode.The wellmatched electrocatalytic property of the electrozyme permits oxidization of reduced nicotinamide adenine dinucleotide(NADH)to release protons under a much lower electric potential.As a consequence,the generated proton gradient drives rotary catalysis of adenosine 5′-triphosphate(ATP)synthase reconstituted in a lipid membrane to produce ATP.Remarkably,electrochemical bioenergy conversion of NADH to ATP is accomplished with much higher efficiency in such a bio-like system compared with the natural mitochondria.This work integrates synthetic and natural catalytic chemistry to facilitate enhanced bioenergy transformation,thereby greatly improving prospects in ATP-fueled bioapplications.
基金The authors gratefully acknowledge the financial support for this research from the National Nature Science Foundation of China(nos.21961142022,21872150,and 22072160)J.F.particularly thanks to the Youth Innovation Promotion Association of CAS(no.2016032)Institute of Chemistry,CAS(no.Y6290512B1).
文摘The manipulation of supramolecular assembly enables single-component architectures to possess diverse structures and functions.Here,we report directed phase transitions of dipeptide supramolecular gel to crystals with excellent selectivity and tunable mechanical properties.To be specific,lamellar-to-orthorhombic rearrangement of dipeptide molecules in the supramolecular assembly was guided by application of ammonia gas,while lamellar-tohexagonal realignment was generated upon water vapor exposure of the assembly.Importantly,this crystal phase control originated from distinct gas-mediated reconstitution of hydrogen-bonding interactions,which endowed the dipeptide materials with remarkably modulated stiffness.The selective phase transformation offers a simple and effective platform for self-assembling peptide crystals with diverse long-range-ordered structures from a single gel-state aggregation.This work opens up new perspectives on peptide-based biomaterials via gas-directed hydrogen-bonding chemistry.
基金the financial support for this research from the National Natural Science Foundation of China(Nos.221930301,21961142022,21872150,and 22072160)J.F.particularly thanks to the Youth Innovation Promotion Association of CAS(No.2016032)Instituteof Chemistry,CAS(No.Y6290512B1).
文摘We construct a natural-artificial hybrid architecture containing black phosphorus nanosheets(BPNS)to enhance photosynthesis of chloroplast in a positive-feedback manner.In this architecture,oxygen yielded by photosynthesis during water splitting by photosystemⅡpromotes the photoreaction of BPNS to produce proton and inorganic phosphate(Pi).Further,transmembrane proton gradient is increased to drive ATP synthase to synthesize ATP.Meanwhile,additional photogenerated electrons produced by BPNS are transferred to the photosynthesis process.As a consequence,photosynthesis performed by chloroplast is improved.Quantitatively,photophosphorylation efficacy of the hybrid system is increased by 1.89 times in the case of Pi deficiency.This work offers a new path to enhance solar-to-chemical energy conversion,holding promise in boosting natural photosynthesis.
